Determination of Quantum Chemistry Based Force Fields for Molecular Dynamics Simulations of Aromatic Polymers

NASA Technical Reports Server (NTRS)

Jaffe, Richard; Langhoff, Stephen R. (Technical Monitor)

1995-01-01

Ab initio quantum chemistry calculations for model molecules can be used to parameterize force fields for molecular dynamics simulations of polymers. Emphasis in our research group is on using quantum chemistry-based force fields for molecular dynamics simulations of organic polymers in the melt and glassy states, but the methodology is applicable to simulations of small molecules, multicomponent systems and solutions. Special attention is paid to deriving reliable descriptions of the non-bonded and electrostatic interactions. Several procedures have been developed for deriving and calibrating these parameters. Our force fields for aromatic polyimide simulations will be described. In this application, the intermolecular interactions are the critical factor in determining many properties of the polymer (including its color).

Experimental simulation of decoherence in photonics qudits

PubMed Central

Marques, B.; Matoso, A. A.; Pimenta, W. M.; Gutiérrez-Esparza, A. J.; Santos, M. F.; Pádua, S.

2015-01-01

We experimentally perform the simulation of open quantum dynamics in single-qudit systems. Using a spatial light modulator as a dissipative optical device, we implement dissipative-dynamical maps onto qudits encoded in the transverse momentum of spontaneous parametric down-converted photon pairs. We show a well-controlled technique to prepare entangled qudits states as well as to implement dissipative local measurements; the latter realize two specific dynamics: dephasing and amplitude damping. Our work represents a new analogy-dynamical experiment for simulating an open quantum system. PMID:26527330

Digital Quantum Simulation of Z2 Lattice Gauge Theories with Dynamical Fermionic Matter

NASA Astrophysics Data System (ADS)

Zohar, Erez; Farace, Alessandro; Reznik, Benni; Cirac, J. Ignacio

2017-02-01

We propose a scheme for digital quantum simulation of lattice gauge theories with dynamical fermions. Using a layered optical lattice with ancilla atoms that can move and interact with the other atoms (simulating the physical degrees of freedom), we obtain a stroboscopic dynamics which yields the four-body plaquette interactions, arising in models with (2 +1 ) and higher dimensions, without the use of perturbation theory. As an example we show how to simulate a Z2 model in (2 +1 ) dimensions.

Digital Quantum Simulation of Z_{2} Lattice Gauge Theories with Dynamical Fermionic Matter.

PubMed

Zohar, Erez; Farace, Alessandro; Reznik, Benni; Cirac, J Ignacio

2017-02-17

We propose a scheme for digital quantum simulation of lattice gauge theories with dynamical fermions. Using a layered optical lattice with ancilla atoms that can move and interact with the other atoms (simulating the physical degrees of freedom), we obtain a stroboscopic dynamics which yields the four-body plaquette interactions, arising in models with (2+1) and higher dimensions, without the use of perturbation theory. As an example we show how to simulate a Z_{2} model in (2+1) dimensions.

Digital Quantum Simulation of Minimal AdS/CFT.

PubMed

García-Álvarez, L; Egusquiza, I L; Lamata, L; Del Campo, A; Sonner, J; Solano, E

2017-07-28

We propose the digital quantum simulation of a minimal AdS/CFT model in controllable quantum platforms. We consider the Sachdev-Ye-Kitaev model describing interacting Majorana fermions with randomly distributed all-to-all couplings, encoding nonlocal fermionic operators onto qubits to efficiently implement their dynamics via digital techniques. Moreover, we also give a method for probing nonequilibrium dynamics and the scrambling of information. Finally, our approach serves as a protocol for reproducing a simplified low-dimensional model of quantum gravity in advanced quantum platforms as trapped ions and superconducting circuits.

Digital Quantum Simulation of Minimal AdS /CFT

NASA Astrophysics Data System (ADS)

García-Álvarez, L.; Egusquiza, I. L.; Lamata, L.; del Campo, A.; Sonner, J.; Solano, E.

2017-07-01

We propose the digital quantum simulation of a minimal AdS /CFT model in controllable quantum platforms. We consider the Sachdev-Ye-Kitaev model describing interacting Majorana fermions with randomly distributed all-to-all couplings, encoding nonlocal fermionic operators onto qubits to efficiently implement their dynamics via digital techniques. Moreover, we also give a method for probing nonequilibrium dynamics and the scrambling of information. Finally, our approach serves as a protocol for reproducing a simplified low-dimensional model of quantum gravity in advanced quantum platforms as trapped ions and superconducting circuits.

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.

Quantum Spin Glasses, Annealing and Computation

NASA Astrophysics Data System (ADS)

Chakrabarti, Bikas K.; Inoue, Jun-ichi; Tamura, Ryo; Tanaka, Shu

2017-05-01

List of tables; List of figures, Preface; 1. Introduction; Part I. Quantum Spin Glass, Annealing and Computation: 2. Classical spin models from ferromagnetic spin systems to spin glasses; 3. Simulated annealing; 4. Quantum spin glass; 5. Quantum dynamics; 6. Quantum annealing; Part II. Additional Notes: 7. Notes on adiabatic quantum computers; 8. Quantum information and quenching dynamics; 9. A brief historical note on the studies of quantum glass, annealing and computation.

On the importance of an accurate representation of the initial state of the system in classical dynamics simulations

NASA Astrophysics Data System (ADS)

García-Vela, A.

2000-05-01

A definition of a quantum-type phase-space distribution is proposed in order to represent the initial state of the system in a classical dynamics simulation. The central idea is to define an initial quantum phase-space state of the system as the direct product of the coordinate and momentum representations of the quantum initial state. The phase-space distribution is then obtained as the square modulus of this phase-space state. The resulting phase-space distribution closely resembles the quantum nature of the system initial state. The initial conditions are sampled with the distribution, using a grid technique in phase space. With this type of sampling the distribution of initial conditions reproduces more faithfully the shape of the original phase-space distribution. The method is applied to generate initial conditions describing the three-dimensional state of the Ar-HCl cluster prepared by ultraviolet excitation. The photodissociation dynamics is simulated by classical trajectories, and the results are compared with those of a wave packet calculation. The classical and quantum descriptions are found in good agreement for those dynamical events less subject to quantum effects. The classical result fails to reproduce the quantum mechanical one for the more strongly quantum features of the dynamics. The properties and applicability of the phase-space distribution and the sampling technique proposed are discussed.

Entanglement dynamics in critical random quantum Ising chain with perturbations

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

Huang, Yichen, E-mail: ychuang@caltech.edu

We simulate the entanglement dynamics in a critical random quantum Ising chain with generic perturbations using the time-evolving block decimation algorithm. Starting from a product state, we observe super-logarithmic growth of entanglement entropy with time. The numerical result is consistent with the analytical prediction of Vosk and Altman using a real-space renormalization group technique. - Highlights: • We study the dynamical quantum phase transition between many-body localized phases. • We simulate the dynamics of a very long random spin chain with matrix product states. • We observe numerically super-logarithmic growth of entanglement entropy with time.

Photonic simulation of entanglement growth and engineering after a spin chain quench.

PubMed

Pitsios, Ioannis; Banchi, Leonardo; Rab, Adil S; Bentivegna, Marco; Caprara, Debora; Crespi, Andrea; Spagnolo, Nicolò; Bose, Sougato; Mataloni, Paolo; Osellame, Roberto; Sciarrino, Fabio

2017-11-17

The time evolution of quantum many-body systems is one of the most important processes for benchmarking quantum simulators. The most curious feature of such dynamics is the growth of quantum entanglement to an amount proportional to the system size (volume law) even when interactions are local. This phenomenon has great ramifications for fundamental aspects, while its optimisation clearly has an impact on technology (e.g., for on-chip quantum networking). Here we use an integrated photonic chip with a circuit-based approach to simulate the dynamics of a spin chain and maximise the entanglement generation. The resulting entanglement is certified by constructing a second chip, which measures the entanglement between multiple distant pairs of simulated spins, as well as the block entanglement entropy. This is the first photonic simulation and optimisation of the extensive growth of entanglement in a spin chain, and opens up the use of photonic circuits for optimising quantum devices.

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.

WavePacket: A Matlab package for numerical quantum dynamics. I: Closed quantum systems and discrete variable representations

NASA Astrophysics Data System (ADS)

Schmidt, Burkhard; Lorenz, Ulf

2017-04-01

WavePacket is an open-source program package for the numerical simulation of quantum-mechanical dynamics. It can be used to solve time-independent or time-dependent linear Schrödinger and Liouville-von Neumann-equations in one or more dimensions. Also coupled equations can be treated, which allows to simulate molecular quantum dynamics beyond the Born-Oppenheimer approximation. Optionally accounting for the interaction with external electric fields within the semiclassical dipole approximation, WavePacket can be used to simulate experiments involving tailored light pulses in photo-induced physics or chemistry. The graphical capabilities allow visualization of quantum dynamics 'on the fly', including Wigner phase space representations. Being easy to use and highly versatile, WavePacket is well suited for the teaching of quantum mechanics as well as for research projects in atomic, molecular and optical physics or in physical or theoretical chemistry. The present Part I deals with the description of closed quantum systems in terms of Schrödinger equations. The emphasis is on discrete variable representations for spatial discretization as well as various techniques for temporal discretization. The upcoming Part II will focus on open quantum systems and dimension reduction; it also describes the codes for optimal control of quantum dynamics. The present work introduces the MATLAB version of WavePacket 5.2.1 which is hosted at the Sourceforge platform, where extensive Wiki-documentation as well as worked-out demonstration examples can be found.

Quantum dynamical simulations of local field enhancement in metal nanoparticles.

PubMed

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

2013-03-27

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

Experimental Trapped-ion Quantum Simulation of the Kibble-Zurek dynamics in momentum space

PubMed Central

Cui, Jin-Ming; Huang, Yun-Feng; Wang, Zhao; Cao, Dong-Yang; Wang, Jian; Lv, Wei-Min; Luo, Le; del Campo, Adolfo; Han, Yong-Jian; Li, Chuan-Feng; Guo, Guang-Can

2016-01-01

The Kibble-Zurek mechanism is the paradigm to account for the nonadiabatic dynamics of a system across a continuous phase transition. Its study in the quantum regime is hindered by the requisite of ground state cooling. We report the experimental quantum simulation of critical dynamics in the transverse-field Ising model by a set of Landau-Zener crossings in pseudo-momentum space, that can be probed with high accuracy using a single trapped ion. We test the Kibble-Zurek mechanism in the quantum regime in the momentum space and find the measured scaling of excitations is in accordance with the theoretical prediction. PMID:27633087

Simulating Open Quantum Systems with Hamiltonian Ensembles and the Nonclassicality of the Dynamics

NASA Astrophysics Data System (ADS)

Chen, Hong-Bin; Gneiting, Clemens; Lo, Ping-Yuan; Chen, Yueh-Nan; Nori, Franco

2018-01-01

The incoherent dynamical properties of open quantum systems are generically attributed to an ongoing correlation between the system and its environment. Here, we propose a novel way to assess the nature of these system-environment correlations by examining the system dynamics alone. Our approach is based on the possibility or impossibility to simulate open-system dynamics with Hamiltonian ensembles. As we show, such (im)possibility to simulate is closely linked to the system-environment correlations. We thus define the nonclassicality of open-system dynamics in terms of the nonexistence of a Hamiltonian-ensemble simulation. This classifies any nonunital open-system dynamics as nonclassical. We give examples for open-system dynamics that are unital and classical, as well as unital and nonclassical.

Mapping quantum-classical Liouville equation: projectors and trajectories.

PubMed

Kelly, Aaron; van Zon, Ramses; Schofield, Jeremy; Kapral, Raymond

2012-02-28

The evolution of a mixed quantum-classical system is expressed in the mapping formalism where discrete quantum states are mapped onto oscillator states, resulting in a phase space description of the quantum degrees of freedom. By defining projection operators onto the mapping states corresponding to the physical quantum states, it is shown that the mapping quantum-classical Liouville operator commutes with the projection operator so that the dynamics is confined to the physical space. It is also shown that a trajectory-based solution of this equation can be constructed that requires the simulation of an ensemble of entangled trajectories. An approximation to this evolution equation which retains only the Poisson bracket contribution to the evolution operator does admit a solution in an ensemble of independent trajectories but it is shown that this operator does not commute with the projection operators and the dynamics may take the system outside the physical space. The dynamical instabilities, utility, and domain of validity of this approximate dynamics are discussed. The effects are illustrated by simulations on several quantum systems.

Detailed Balance of Thermalization Dynamics in Rydberg-Atom Quantum Simulators.

PubMed

Kim, Hyosub; Park, YeJe; Kim, Kyungtae; Sim, H-S; Ahn, Jaewook

2018-05-04

Dynamics of large complex systems, such as relaxation towards equilibrium in classical statistical mechanics, often obeys a master equation that captures essential information from the complexities. Here, we find that thermalization of an isolated many-body quantum state can be described by a master equation. We observe sudden quench dynamics of quantum Ising-like models implemented in our quantum simulator, defect-free single-atom tweezers in conjunction with Rydberg-atom interaction. Saturation of their local observables, a thermalization signature, obeys a master equation experimentally constructed by monitoring the occupation probabilities of prequench states and imposing the principle of the detailed balance. Our experiment agrees with theories and demonstrates the detailed balance in a thermalization dynamics that does not require coupling to baths or postulated randomness.

Detailed Balance of Thermalization Dynamics in Rydberg-Atom Quantum Simulators

NASA Astrophysics Data System (ADS)

Kim, Hyosub; Park, YeJe; Kim, Kyungtae; Sim, H.-S.; Ahn, Jaewook

2018-05-01

Dynamics of large complex systems, such as relaxation towards equilibrium in classical statistical mechanics, often obeys a master equation that captures essential information from the complexities. Here, we find that thermalization of an isolated many-body quantum state can be described by a master equation. We observe sudden quench dynamics of quantum Ising-like models implemented in our quantum simulator, defect-free single-atom tweezers in conjunction with Rydberg-atom interaction. Saturation of their local observables, a thermalization signature, obeys a master equation experimentally constructed by monitoring the occupation probabilities of prequench states and imposing the principle of the detailed balance. Our experiment agrees with theories and demonstrates the detailed balance in a thermalization dynamics that does not require coupling to baths or postulated randomness.

Path-integral isomorphic Hamiltonian for including nuclear quantum effects in non-adiabatic dynamics

NASA Astrophysics Data System (ADS)

Tao, Xuecheng; Shushkov, Philip; Miller, Thomas F.

2018-03-01

We describe a path-integral approach for including nuclear quantum effects in non-adiabatic chemical dynamics simulations. For a general physical system with multiple electronic energy levels, a corresponding isomorphic Hamiltonian is introduced such that Boltzmann sampling of the isomorphic Hamiltonian with classical nuclear degrees of freedom yields the exact quantum Boltzmann distribution for the original physical system. In the limit of a single electronic energy level, the isomorphic Hamiltonian reduces to the familiar cases of either ring polymer molecular dynamics (RPMD) or centroid molecular dynamics Hamiltonians, depending on the implementation. An advantage of the isomorphic Hamiltonian is that it can easily be combined with existing mixed quantum-classical dynamics methods, such as surface hopping or Ehrenfest dynamics, to enable the simulation of electronically non-adiabatic processes with nuclear quantum effects. We present numerical applications of the isomorphic Hamiltonian to model two- and three-level systems, with encouraging results that include improvement upon a previously reported combination of RPMD with surface hopping in the deep-tunneling regime.

Dynamics of Topological Excitations in a Model Quantum Spin Ice

NASA Astrophysics Data System (ADS)

Huang, Chun-Jiong; Deng, Youjin; Wan, Yuan; Meng, Zi Yang

2018-04-01

We study the quantum spin dynamics of a frustrated X X Z model on a pyrochlore lattice by using large-scale quantum Monte Carlo simulation and stochastic analytic continuation. In the low-temperature quantum spin ice regime, we observe signatures of coherent photon and spinon excitations in the dynamic spin structure factor. As the temperature rises to the classical spin ice regime, the photon disappears from the dynamic spin structure factor, whereas the dynamics of the spinon remain coherent in a broad temperature window. Our results provide experimentally relevant, quantitative information for the ongoing pursuit of quantum spin ice materials.

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

Atomic quantum simulation of dynamical gauge fields coupled to fermionic matter: from string breaking to evolution after a quench.

PubMed

Banerjee, D; Dalmonte, M; Müller, M; Rico, E; Stebler, P; Wiese, U-J; Zoller, P

2012-10-26

Using a Fermi-Bose mixture of ultracold atoms in an optical lattice, we construct a quantum simulator for a U(1) gauge theory coupled to fermionic matter. The construction is based on quantum links which realize continuous gauge symmetry with discrete quantum variables. At low energies, quantum link models with staggered fermions emerge from a Hubbard-type model which can be quantum simulated. This allows us to investigate string breaking as well as the real-time evolution after a quench in gauge theories, which are inaccessible to classical simulation methods.

Towards photonic quantum simulation of ground states of frustrated Heisenberg spin systems

PubMed Central

Ma, Xiao-song; Dakić, Borivoje; Kropatschek, Sebastian; Naylor, William; Chan, Yang-hao; Gong, Zhe-xuan; Duan, Lu-ming; Zeilinger, Anton; Walther, Philip

2014-01-01

Photonic quantum simulators are promising candidates for providing insight into other small- to medium-sized quantum systems. Recent experiments have shown that photonic quantum systems have the advantage to exploit quantum interference for the quantum simulation of the ground state of Heisenberg spin systems. Here we experimentally characterize this quantum interference at a tuneable beam splitter and further investigate the measurement-induced interactions of a simulated four-spin system by comparing the entanglement dynamics using pairwise concurrence. We also study theoretically a four-site square lattice with next-nearest neighbor interactions and a six-site checkerboard lattice, which might be in reach of current technology. PMID:24394808

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.

Simulating chemistry using quantum computers.

PubMed

Kassal, Ivan; Whitfield, James D; Perdomo-Ortiz, Alejandro; Yung, Man-Hong; Aspuru-Guzik, Alán

2011-01-01

The difficulty of simulating quantum systems, well known to quantum chemists, prompted the idea of quantum computation. One can avoid the steep scaling associated with the exact simulation of increasingly large quantum systems on conventional computers, by mapping the quantum system to another, more controllable one. In this review, we discuss to what extent the ideas in quantum computation, now a well-established field, have been applied to chemical problems. We describe algorithms that achieve significant advantages for the electronic-structure problem, the simulation of chemical dynamics, protein folding, and other tasks. Although theory is still ahead of experiment, we outline recent advances that have led to the first chemical calculations on small quantum information processors.

Quantum chemistry simulation on quantum computers: theories and experiments.

PubMed

Lu, Dawei; Xu, Boruo; Xu, Nanyang; Li, Zhaokai; Chen, Hongwei; Peng, Xinhua; Xu, Ruixue; Du, Jiangfeng

2012-07-14

It has been claimed that quantum computers can mimic quantum systems efficiently in the polynomial scale. Traditionally, those simulations are carried out numerically on classical computers, which are inevitably confronted with the exponential growth of required resources, with the increasing size of quantum systems. Quantum computers avoid this problem, and thus provide a possible solution for large quantum systems. In this paper, we first discuss the ideas of quantum simulation, the background of quantum simulators, their categories, and the development in both theories and experiments. We then present a brief introduction to quantum chemistry evaluated via classical computers followed by typical procedures of quantum simulation towards quantum chemistry. Reviewed are not only theoretical proposals but also proof-of-principle experimental implementations, via a small quantum computer, which include the evaluation of the static molecular eigenenergy and the simulation of chemical reaction dynamics. Although the experimental development is still behind the theory, we give prospects and suggestions for future experiments. We anticipate that in the near future quantum simulation will become a powerful tool for quantum chemistry over classical computations.

Classical simulation of quantum error correction in a Fibonacci anyon code

NASA Astrophysics Data System (ADS)

Burton, Simon; Brell, Courtney G.; Flammia, Steven T.

2017-02-01

Classically simulating the dynamics of anyonic excitations in two-dimensional quantum systems is likely intractable in general because such dynamics are sufficient to implement universal quantum computation. However, processes of interest for the study of quantum error correction in anyon systems are typically drawn from a restricted class that displays significant structure over a wide range of system parameters. We exploit this structure to classically simulate, and thereby demonstrate the success of, an error-correction protocol for a quantum memory based on the universal Fibonacci anyon model. We numerically simulate a phenomenological model of the system and noise processes on lattice sizes of up to 128 ×128 sites, and find a lower bound on the error-correction threshold of approximately 0.125 errors per edge, which is comparable to those previously known for Abelian and (nonuniversal) non-Abelian anyon models.

Full Quantum Dynamics Simulation of a Realistic Molecular System Using the Adaptive Time-Dependent Density Matrix Renormalization Group Method.

PubMed

Yao, Yao; Sun, Ke-Wei; Luo, Zhen; Ma, Haibo

2018-01-18

The accurate theoretical interpretation of ultrafast time-resolved spectroscopy experiments relies on full quantum dynamics simulations for the investigated system, which is nevertheless computationally prohibitive for realistic molecular systems with a large number of electronic and/or vibrational degrees of freedom. In this work, we propose a unitary transformation approach for realistic vibronic Hamiltonians, which can be coped with using the adaptive time-dependent density matrix renormalization group (t-DMRG) method to efficiently evolve the nonadiabatic dynamics of a large molecular system. We demonstrate the accuracy and efficiency of this approach with an example of simulating the exciton dissociation process within an oligothiophene/fullerene heterojunction, indicating that t-DMRG can be a promising method for full quantum dynamics simulation in large chemical systems. Moreover, it is also shown that the proper vibronic features in the ultrafast electronic process can be obtained by simulating the two-dimensional (2D) electronic spectrum by virtue of the high computational efficiency of the t-DMRG method.

Quantum simulation of ultrafast dynamics using trapped ultracold atoms.

PubMed

Senaratne, Ruwan; Rajagopal, Shankari V; Shimasaki, Toshihiko; Dotti, Peter E; Fujiwara, Kurt M; Singh, Kevin; Geiger, Zachary A; Weld, David M

2018-05-25

Ultrafast electronic dynamics are typically studied using pulsed lasers. Here we demonstrate a complementary experimental approach: quantum simulation of ultrafast dynamics using trapped ultracold atoms. Counter-intuitively, this technique emulates some of the fastest processes in atomic physics with some of the slowest, leading to a temporal magnification factor of up to 12 orders of magnitude. In these experiments, time-varying forces on neutral atoms in the ground state of a tunable optical trap emulate the electric fields of a pulsed laser acting on bound charged particles. We demonstrate the correspondence with ultrafast science by a sequence of experiments: nonlinear spectroscopy of a many-body bound state, control of the excitation spectrum by potential shaping, observation of sub-cycle unbinding dynamics during strong few-cycle pulses, and direct measurement of carrier-envelope phase dependence of the response to an ultrafast-equivalent pulse. These results establish cold-atom quantum simulation as a complementary tool for studying ultrafast dynamics.

Emulation of complex open quantum systems using superconducting qubits

NASA Astrophysics Data System (ADS)

Mostame, Sarah; Huh, Joonsuk; Kreisbeck, Christoph; Kerman, Andrew J.; Fujita, Takatoshi; Eisfeld, Alexander; Aspuru-Guzik, Alán

2017-02-01

With quantum computers being out of reach for now, quantum simulators are alternative devices for efficient and accurate simulation of problems that are challenging to tackle using conventional computers. Quantum simulators are classified into analog and digital, with the possibility of constructing "hybrid" simulators by combining both techniques. Here we focus on analog quantum simulators of open quantum systems and address the limit that they can beat classical computers. In particular, as an example, we discuss simulation of the chlorosome light-harvesting antenna from green sulfur bacteria with over 250 phonon modes coupled to each electronic state. Furthermore, we propose physical setups that can be used to reproduce the quantum dynamics of a standard and multiple-mode Holstein model. The proposed scheme is based on currently available technology of superconducting circuits consist of flux qubits and quantum oscillators.

Stochastic wave-function simulation of irreversible emission processes for open quantum systems in a non-Markovian environment

NASA Astrophysics Data System (ADS)

Polyakov, Evgeny A.; Rubtsov, Alexey N.

2018-02-01

When conducting the numerical simulation of quantum transport, the main obstacle is a rapid growth of the dimension of entangled Hilbert subspace. The Quantum Monte Carlo simulation techniques, while being capable of treating the problems of high dimension, are hindered by the so-called "sign problem". In the quantum transport, we have fundamental asymmetry between the processes of emission and absorption of environment excitations: the emitted excitations are rapidly and irreversibly scattered away. Whereas only a small part of these excitations is absorbed back by the open subsystem, thus exercising the non-Markovian self-action of the subsystem onto itself. We were able to devise a method for the exact simulation of the dominant quantum emission processes, while taking into account the small backaction effects in an approximate self-consistent way. Such an approach allows us to efficiently conduct simulations of real-time dynamics of small quantum subsystems immersed in non-Markovian bath for large times, reaching the quasistationary regime. As an example we calculate the spatial quench dynamics of Kondo cloud for a bozonized Kodno impurity model.

Quantum Monte Carlo tunneling from quantum chemistry to quantum annealing

NASA Astrophysics Data System (ADS)

Mazzola, Guglielmo; Smelyanskiy, Vadim N.; Troyer, Matthias

2017-10-01

Quantum tunneling is ubiquitous across different fields, from quantum chemical reactions and magnetic materials to quantum simulators and quantum computers. While simulating the real-time quantum dynamics of tunneling is infeasible for high-dimensional systems, quantum tunneling also shows up in quantum Monte Carlo (QMC) simulations, which aim to simulate quantum statistics with resources growing only polynomially with the system size. Here we extend the recent results obtained for quantum spin models [Phys. Rev. Lett. 117, 180402 (2016), 10.1103/PhysRevLett.117.180402], and we study continuous-variable models for proton transfer reactions. We demonstrate that QMC simulations efficiently recover the scaling of ground-state tunneling rates due to the existence of an instanton path, which always connects the reactant state with the product. We discuss the implications of our results in the context of quantum chemical reactions and quantum annealing, where quantum tunneling is expected to be a valuable resource for solving combinatorial optimization problems.

Reproducing Quantum Probability Distributions at the Speed of Classical Dynamics: A New Approach for Developing Force-Field Functors.

PubMed

Sundar, Vikram; Gelbwaser-Klimovsky, David; Aspuru-Guzik, Alán

2018-04-05

Modeling nuclear quantum effects is required for accurate molecular dynamics (MD) simulations of molecules. The community has paid special attention to water and other biomolecules that show hydrogen bonding. Standard methods of modeling nuclear quantum effects like Ring Polymer Molecular Dynamics (RPMD) are computationally costlier than running classical trajectories. A force-field functor (FFF) is an alternative method that computes an effective force field that replicates quantum properties of the original force field. In this work, we propose an efficient method of computing FFF using the Wigner-Kirkwood expansion. As a test case, we calculate a range of thermodynamic properties of Neon, obtaining the same level of accuracy as RPMD, but with the shorter runtime of classical simulations. By modifying existing MD programs, the proposed method could be used in the future to increase the efficiency and accuracy of MD simulations involving water and proteins.

Quantum critical probing and simulation of colored quantum noise

NASA Astrophysics Data System (ADS)

Mascarenhas, Eduardo; de Vega, Inés

2017-12-01

We propose a protocol to simulate the evolution of a non-Markovian open quantum system by considering a collisional process with a many-body system, which plays the role of an environment. As a result of our protocol, the environment spatial correlations are mapped into the time correlations of a noise that drives the dynamics of the open system. Considering the weak coupling limit, the open system can also be considered as a probe of the environment properties. In this regard, when preparing the environment in its ground state, a measurement of the dynamics of the open system allows to determine the length of the environment spatial correlations and therefore its critical properties. To illustrate our proposal we simulate the full system dynamics with matrix-product-states and compare this to the reduced dynamics obtained with an approximated variational master equation.

Nonadiabatic Dynamics in Single-Electron Tunneling Devices with Time-Dependent Density-Functional Theory

NASA Astrophysics Data System (ADS)

Dittmann, Niklas; Splettstoesser, Janine; Helbig, Nicole

2018-04-01

We simulate the dynamics of a single-electron source, modeled as a quantum dot with on-site Coulomb interaction and tunnel coupling to an adjacent lead in time-dependent density-functional theory. Based on this system, we develop a time-nonlocal exchange-correlation potential by exploiting analogies with quantum-transport theory. The time nonlocality manifests itself in a dynamical potential step. We explicitly link the time evolution of the dynamical step to physical relaxation timescales of the electron dynamics. Finally, we discuss prospects for simulations of larger mesoscopic systems.

Nonadiabatic Dynamics in Single-Electron Tunneling Devices with Time-Dependent Density-Functional Theory.

PubMed

Dittmann, Niklas; Splettstoesser, Janine; Helbig, Nicole

2018-04-13

We simulate the dynamics of a single-electron source, modeled as a quantum dot with on-site Coulomb interaction and tunnel coupling to an adjacent lead in time-dependent density-functional theory. Based on this system, we develop a time-nonlocal exchange-correlation potential by exploiting analogies with quantum-transport theory. The time nonlocality manifests itself in a dynamical potential step. We explicitly link the time evolution of the dynamical step to physical relaxation timescales of the electron dynamics. Finally, we discuss prospects for simulations of larger mesoscopic systems.

Hybrid classical/quantum simulation for infrared spectroscopy of water

NASA Astrophysics Data System (ADS)

Maekawa, Yuki; Sasaoka, Kenji; Ube, Takuji; Ishiguro, Takashi; Yamamoto, Takahiro

2018-05-01

We have developed a hybrid classical/quantum simulation method to calculate the infrared (IR) spectrum of water. The proposed method achieves much higher accuracy than conventional classical molecular dynamics (MD) simulations at a much lower computational cost than ab initio MD simulations. The IR spectrum of water is obtained as an ensemble average of the eigenvalues of the dynamical matrix constructed by ab initio calculations, using the positions of oxygen atoms that constitute water molecules obtained from the classical MD simulation. The calculated IR spectrum is in excellent agreement with the experimental IR spectrum.

Using time reversal to detect entanglement and spreading of quantum information

NASA Astrophysics Data System (ADS)

Gaerttner, Martin

2017-04-01

Characterizing and understanding the states of interacting quantum systems and their non-equilibrium dynamics is the goal of quantum simulation. For this it is crucial to find experimentally feasible means for quantifying how entanglement and correlation build up and spread. The ability of analog quantum simulators to reverse the unitary dynamics of quantum many-body systems provides new tools in this quest. One such tool is the multiple-quantum coherence (MQC) spectrum previously used in NMR spectroscopy which can now be studied in so far inaccessible parameter regimes near zero temperature in highly controllable environments. I present recent progress in relating the MQC spectrum to established entanglement witnesses such as quantum Fisher information. Recognizing the MQC as out-of-time-order correlation functions, which quantify the spreading, or scrambling, of quantum information, allows us to establish a connection between these quantities and multi-partite entanglement. I will show recent experimental results obtained with a trapped ion quantum simulator and a spinor BEC illustrating the power of time reversal protocols. Supported by: JILA-NSF-PFC-1125844, NSF-PHY-1521080, ARO, AFOSR, AFOSR-MURI, DARPA, NIST.

A Generic Simulation Framework for Non-Entangled based Experimental Quantum Cryptography and Communication: Quantum Cryptography and Communication Simulator (QuCCs)

NASA Astrophysics Data System (ADS)

Buhari, Abudhahir; Zukarnain, Zuriati Ahmad; Khalid, Roszelinda; Zakir Dato', Wira Jaafar Ahmad

2016-11-01

The applications of quantum information science move towards bigger and better heights for the next generation technology. Especially, in the field of quantum cryptography and quantum computation, the world already witnessed various ground-breaking tangible product and promising results. Quantum cryptography is one of the mature field from quantum mechanics and already available in the markets. The current state of quantum cryptography is still under various researches in order to reach the heights of digital cryptography. The complexity of quantum cryptography is higher due to combination of hardware and software. The lack of effective simulation tool to design and analyze the quantum cryptography experiments delays the reaching distance of the success. In this paper, we propose a framework to achieve an effective non-entanglement based quantum cryptography simulation tool. We applied hybrid simulation technique i.e. discrete event, continuous event and system dynamics. We also highlight the limitations of a commercial photonic simulation tool based experiments. Finally, we discuss ideas for achieving one-stop simulation package for quantum based secure key distribution experiments. All the modules of simulation framework are viewed from the computer science perspective.

Higher-order spin and charge dynamics in a quantum dot-lead hybrid system.

PubMed

Otsuka, Tomohiro; Nakajima, Takashi; Delbecq, Matthieu R; Amaha, Shinichi; Yoneda, Jun; Takeda, Kenta; Allison, Giles; Stano, Peter; Noiri, Akito; Ito, Takumi; Loss, Daniel; Ludwig, Arne; Wieck, Andreas D; Tarucha, Seigo

2017-09-22

Understanding the dynamics of open quantum systems is important and challenging in basic physics and applications for quantum devices and quantum computing. Semiconductor quantum dots offer a good platform to explore the physics of open quantum systems because we can tune parameters including the coupling to the environment or leads. Here, we apply the fast single-shot measurement techniques from spin qubit experiments to explore the spin and charge dynamics due to tunnel coupling to a lead in a quantum dot-lead hybrid system. We experimentally observe both spin and charge time evolution via first- and second-order tunneling processes, and reveal the dynamics of the spin-flip through the intermediate state. These results enable and stimulate the exploration of spin dynamics in dot-lead hybrid systems, and may offer useful resources for spin manipulation and simulation of open quantum systems.

Analog quantum simulation of the Rabi model in the ultra-strong coupling regime.

PubMed

Braumüller, Jochen; Marthaler, Michael; Schneider, Andre; Stehli, Alexander; Rotzinger, Hannes; Weides, Martin; Ustinov, Alexey V

2017-10-03

The quantum Rabi model describes the fundamental mechanism of light-matter interaction. It consists of a two-level atom or qubit coupled to a quantized harmonic mode via a transversal interaction. In the weak coupling regime, it reduces to the well-known Jaynes-Cummings model by applying a rotating wave approximation. The rotating wave approximation breaks down in the ultra-strong coupling regime, where the effective coupling strength g is comparable to the energy ω of the bosonic mode, and remarkable features in the system dynamics are revealed. Here we demonstrate an analog quantum simulation of an effective quantum Rabi model in the ultra-strong coupling regime, achieving a relative coupling ratio of g/ω ~ 0.6. The quantum hardware of the simulator is a superconducting circuit embedded in a cQED setup. We observe fast and periodic quantum state collapses and revivals of the initial qubit state, being the most distinct signature of the synthesized model.An analog quantum simulation scheme has been explored with a quantum hardware based on a superconducting circuit. Here the authors investigate the time evolution of the quantum Rabi model at ultra-strong coupling conditions, which is synthesized by slowing down the system dynamics in an effective frame.

Quantum Monte Carlo Methods for First Principles Simulation of Liquid Water

ERIC Educational Resources Information Center

Gergely, John Robert

2009-01-01

Obtaining an accurate microscopic description of water structure and dynamics is of great interest to molecular biology researchers and in the physics and quantum chemistry simulation communities. This dissertation describes efforts to apply quantum Monte Carlo methods to this problem with the goal of making progress toward a fully "ab initio"…

Quantum simulation of disordered systems with cold atoms

NASA Astrophysics Data System (ADS)

Garreau, Jean-Claude

2017-01-01

This paper reviews the physics of quantum disorder in relation with a series of experiments using laser-cooled atoms exposed to "kicks" of a standing wave, realizing a paradigmatic model of quantum chaos, the kicked rotor. This dynamical system can be mapped onto a tight-binding Hamiltonian with pseudo-disorder, formally equivalent to the Anderson model of quantum disorder, with quantum chaos playing the role of disorder. This provides a very good quantum simulator for the Anderson physics. xml:lang="fr"

Revealing missing charges with generalised quantum fluctuation relations.

PubMed

Mur-Petit, J; Relaño, A; Molina, R A; Jaksch, D

2018-05-22

The non-equilibrium dynamics of quantum many-body systems is one of the most fascinating problems in physics. Open questions range from how they relax to equilibrium to how to extract useful work from them. A critical point lies in assessing whether a system has conserved quantities (or 'charges'), as these can drastically influence its dynamics. Here we propose a general protocol to reveal the existence of charges based on a set of exact relations between out-of-equilibrium fluctuations and equilibrium properties of a quantum system. We apply these generalised quantum fluctuation relations to a driven quantum simulator, demonstrating their relevance to obtain unbiased temperature estimates from non-equilibrium measurements. Our findings will help guide research on the interplay of quantum and thermal fluctuations in quantum simulation, in studying the transition from integrability to chaos and in the design of new quantum devices.

Open source Matrix Product States: Opening ways to simulate entangled many-body quantum systems in one dimension

NASA Astrophysics Data System (ADS)

Jaschke, Daniel; Wall, Michael L.; Carr, Lincoln D.

2018-04-01

Numerical simulations are a powerful tool to study quantum systems beyond exactly solvable systems lacking an analytic expression. For one-dimensional entangled quantum systems, tensor network methods, amongst them Matrix Product States (MPSs), have attracted interest from different fields of quantum physics ranging from solid state systems to quantum simulators and quantum computing. Our open source MPS code provides the community with a toolset to analyze the statics and dynamics of one-dimensional quantum systems. Here, we present our open source library, Open Source Matrix Product States (OSMPS), of MPS methods implemented in Python and Fortran2003. The library includes tools for ground state calculation and excited states via the variational ansatz. We also support ground states for infinite systems with translational invariance. Dynamics are simulated with different algorithms, including three algorithms with support for long-range interactions. Convenient features include built-in support for fermionic systems and number conservation with rotational U(1) and discrete Z2 symmetries for finite systems, as well as data parallelism with MPI. We explain the principles and techniques used in this library along with examples of how to efficiently use the general interfaces to analyze the Ising and Bose-Hubbard models. This description includes the preparation of simulations as well as dispatching and post-processing of them.

Experimentally simulating the dynamics of quantum light and matter at ultrastrong coupling using circuit QED (1) - implementation and matter dynamics -

NASA Astrophysics Data System (ADS)

Kounalakis, M.; Langford, N. K.; Sagastizabal, R.; Dickel, C.; Bruno, A.; Luthi, F.; Thoen, D. J.; Endo, A.; Dicarlo, L.

The field dipole coupling of quantum light and matter, described by the quantum Rabi model, leads to exotic phenomena when the coupling strength g becomes comparable or larger than the atom and photon frequencies ωq , r. In this ultra-strong coupling regime, excitations are not conserved, leading to collapse-revival dynamics in atom and photon parity and Schrödinger-cat-like atom-photon entanglement. We realize a quantum simulation of the Rabi model using a transmon qubit coupled to a resonator. In this first part, we describe our analog-digital approach to implement up to 90 symmetric Trotter steps, combining single-qubit gates with the Jaynes-Cummings interaction naturally present in our circuit QED system. Controlling the phase of microwave pulses defines a rotating frame and enables simulation of arbitrary parameter regimes of the Rabi model. We demonstrate measurements of qubit parity dynamics showing revivals at g /ωr > 0 . 8 for ωq = 0 and characteristic dynamics for nondegenerate ωq from g / 4 to g. Funding from the EU FP7 Project ScaleQIT, an ERC Grant, the Dutch Research Organization NWO, and Microsoft Research.

Including Memory Friction in Single- and Two-State Quantum Dynamics Simulations.

PubMed

Brown, Paul A; Messina, Michael

2016-03-03

We present a simple computational algorithm that allows for the inclusion of memory friction in a quantum dynamics simulation of a small, quantum, primary system coupled to many atoms in the surroundings. We show how including a memory friction operator, F̂, in the primary quantum system's Hamiltonian operator builds memory friction into the dynamics of the primary quantum system. We show that, in the harmonic, semi-classical limit, this friction operator causes the classical phase-space centers of a wavepacket to evolve exactly as if it were a classical particle experiencing memory friction. We also show that this friction operator can be used to include memory friction in the quantum dynamics of an anharmonic primary system. We then generalize the algorithm so that it can be used to treat a primary quantum system that is evolving, non-adiabatically on two coupled potential energy surfaces, i.e., a model that can be used to model H atom transfer, for example. We demonstrate this approach's computational ease and flexibility by showing numerical results for both harmonic and anharmonic primary quantum systems in the single surface case. Finally, we present numerical results for a model of non-adiabatic H atom transfer between a reactant and product state that includes memory friction on one or both of the non-adiabatic potential energy surfaces and uncover some interesting dynamical effects of non-memory friction on the H atom transfer process.

Toward simulating complex systems with quantum effects

NASA Astrophysics Data System (ADS)

Kenion-Hanrath, Rachel Lynn

Quantum effects like tunneling, coherence, and zero point energy often play a significant role in phenomena on the scales of atoms and molecules. However, the exact quantum treatment of a system scales exponentially with dimensionality, making it impractical for characterizing reaction rates and mechanisms in complex systems. An ongoing effort in the field of theoretical chemistry and physics is extending scalable, classical trajectory-based simulation methods capable of capturing quantum effects to describe dynamic processes in many-body systems; in the work presented here we explore two such techniques. First, we detail an explicit electron, path integral (PI)-based simulation protocol for predicting the rate of electron transfer in condensed-phase transition metal complex systems. Using a PI representation of the transferring electron and a classical representation of the transition metal complex and solvent atoms, we compute the outer sphere free energy barrier and dynamical recrossing factor of the electron transfer rate while accounting for quantum tunneling and zero point energy effects. We are able to achieve this employing only a single set of force field parameters to describe the system rather than parameterizing along the reaction coordinate. Following our success in describing a simple model system, we discuss our next steps in extending our protocol to technologically relevant materials systems. The latter half focuses on the Mixed Quantum-Classical Initial Value Representation (MQC-IVR) of real-time correlation functions, a semiclassical method which has demonstrated its ability to "tune'' between quantum- and classical-limit correlation functions while maintaining dynamic consistency. Specifically, this is achieved through a parameter that determines the quantumness of individual degrees of freedom. Here, we derive a semiclassical correction term for the MQC-IVR to systematically characterize the error introduced by different choices of simulation parameters, and demonstrate the ability of this approach to optimize MQC-IVR simulations.

Quantum dynamics modeled by interacting trajectories

NASA Astrophysics Data System (ADS)

Cruz-Rodríguez, L.; Uranga-Piña, L.; Martínez-Mesa, A.; Meier, C.

2018-03-01

We present quantum dynamical simulations based on the propagation of interacting trajectories where the effect of the quantum potential is mimicked by effective pseudo-particle interactions. The method is applied to several quantum systems, both for bound and scattering problems. For the bound systems, the quantum ground state density and zero point energy are shown to be perfectly obtained by the interacting trajectories. In the case of time-dependent quantum scattering, the Eckart barrier and uphill ramp are considered, with transmission coefficients in very good agreement with standard quantum calculations. Finally, we show that via wave function synthesis along the trajectories, correlation functions and energy spectra can be obtained based on the dynamics of interacting trajectories.

Simulations of Probabilities for Quantum Computing

NASA Technical Reports Server (NTRS)

Zak, M.

1996-01-01

It has been demonstrated that classical probabilities, and in particular, probabilistic Turing machine, can be simulated by combining chaos and non-LIpschitz dynamics, without utilization of any man-made devices (such as random number generators). Self-organizing properties of systems coupling simulated and calculated probabilities and their link to quantum computations are discussed.

Efficient Measurement of Multiparticle Entanglement with Embedding Quantum Simulator.

PubMed

Chen, Ming-Cheng; Wu, Dian; Su, Zu-En; Cai, Xin-Dong; Wang, Xi-Lin; Yang, Tao; Li, Li; Liu, Nai-Le; Lu, Chao-Yang; Pan, Jian-Wei

2016-02-19

The quantum measurement of entanglement is a demanding task in the field of quantum information. Here, we report the direct and scalable measurement of multiparticle entanglement with embedding photonic quantum simulators. In this embedding framework [R. Di Candia et al. Phys. Rev. Lett. 111, 240502 (2013)], the N-qubit entanglement, which does not associate with a physical observable directly, can be efficiently measured with only two (for even N) and six (for odd N) local measurement settings. Our experiment uses multiphoton quantum simulators to mimic dynamical concurrence and three-tangle entangled systems and to track their entanglement evolutions.

Communication: On the consistency of approximate quantum dynamics simulation methods for vibrational spectra in the condensed phase.

PubMed

Rossi, Mariana; Liu, Hanchao; Paesani, Francesco; Bowman, Joel; Ceriotti, Michele

2014-11-14

Including quantum mechanical effects on the dynamics of nuclei in the condensed phase is challenging, because the complexity of exact methods grows exponentially with the number of quantum degrees of freedom. Efforts to circumvent these limitations can be traced down to two approaches: methods that treat a small subset of the degrees of freedom with rigorous quantum mechanics, considering the rest of the system as a static or classical environment, and methods that treat the whole system quantum mechanically, but using approximate dynamics. Here, we perform a systematic comparison between these two philosophies for the description of quantum effects in vibrational spectroscopy, taking the Embedded Local Monomer model and a mixed quantum-classical model as representatives of the first family of methods, and centroid molecular dynamics and thermostatted ring polymer molecular dynamics as examples of the latter. We use as benchmarks D2O doped with HOD and pure H2O at three distinct thermodynamic state points (ice Ih at 150 K, and the liquid at 300 K and 600 K), modeled with the simple q-TIP4P/F potential energy and dipole moment surfaces. With few exceptions the different techniques yield IR absorption frequencies that are consistent with one another within a few tens of cm(-1). Comparison with classical molecular dynamics demonstrates the importance of nuclear quantum effects up to the highest temperature, and a detailed discussion of the discrepancies between the various methods let us draw some (circumstantial) conclusions about the impact of the very different approximations that underlie them. Such cross validation between radically different approaches could indicate a way forward to further improve the state of the art in simulations of condensed-phase quantum dynamics.

Communication: Quantum molecular dynamics simulation of liquid para-hydrogen by nuclear and electron wave packet approach.

PubMed

Hyeon-Deuk, Kim; Ando, Koji

2014-05-07

Liquid para-hydrogen (p-H2) is a typical quantum liquid which exhibits strong nuclear quantum effects (NQEs) and thus anomalous static and dynamic properties. We propose a real-time simulation method of wave packet (WP) molecular dynamics (MD) based on non-empirical intra- and inter-molecular interactions of non-spherical hydrogen molecules, and apply it to condensed-phase p-H2. The NQEs, such as WP delocalization and zero-point energy, are taken into account without perturbative expansion of prepared model potential functions but with explicit interactions between nuclear and electron WPs. The developed MD simulation for 100 ps with 1200 hydrogen molecules is realized at feasible computational cost, by which basic experimental properties of p-H2 liquid such as radial distribution functions, self-diffusion coefficients, and shear viscosities are all well reproduced.

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.

Next Generation Extended Lagrangian Quantum-based Molecular Dynamics

NASA Astrophysics Data System (ADS)

Negre, Christian

2017-06-01

A new framework for extended Lagrangian first-principles molecular dynamics simulations is presented, which overcomes shortcomings of regular, direct Born-Oppenheimer molecular dynamics, while maintaining important advantages of the unified extended Lagrangian formulation of density functional theory pioneered by Car and Parrinello three decades ago. The new framework allows, for the first time, energy conserving, linear-scaling Born-Oppenheimer molecular dynamics simulations, which is necessary to study larger and more realistic systems over longer simulation times than previously possible. Expensive, self-consinstent-field optimizations are avoided and normal integration time steps of regular, direct Born-Oppenheimer molecular dynamics can be used. Linear scaling electronic structure theory is presented using a graph-based approach that is ideal for parallel calculations on hybrid computer platforms. For the first time, quantum based Born-Oppenheimer molecular dynamics simulation is becoming a practically feasible approach in simulations of +100,000 atoms-representing a competitive alternative to classical polarizable force field methods. In collaboration with: Anders Niklasson, Los Alamos National Laboratory.

Efficient tomography of a quantum many-body system

NASA Astrophysics Data System (ADS)

Lanyon, B. P.; Maier, C.; Holzäpfel, M.; Baumgratz, T.; Hempel, C.; Jurcevic, P.; Dhand, I.; Buyskikh, A. S.; Daley, A. J.; Cramer, M.; Plenio, M. B.; Blatt, R.; Roos, C. F.

2017-12-01

Quantum state tomography is the standard technique for estimating the quantum state of small systems. But its application to larger systems soon becomes impractical as the required resources scale exponentially with the size. Therefore, considerable effort is dedicated to the development of new characterization tools for quantum many-body states. Here we demonstrate matrix product state tomography, which is theoretically proven to allow for the efficient and accurate estimation of a broad class of quantum states. We use this technique to reconstruct the dynamical state of a trapped-ion quantum simulator comprising up to 14 entangled and individually controlled spins: a size far beyond the practical limits of quantum state tomography. Our results reveal the dynamical growth of entanglement and describe its complexity as correlations spread out during a quench: a necessary condition for future demonstrations of better-than-classical performance. Matrix product state tomography should therefore find widespread use in the study of large quantum many-body systems and the benchmarking and verification of quantum simulators and computers.

Communication: Methane dissociation on Ni(111) surface: Importance of azimuth and surface impact site

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

Shen, Xiangjian; State Key Laboratory of Molecular Reaction Dynamics and Center for Theoretical Computational Chemistry, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023; Zhang, Zhaojun, E-mail: zhangzhj@dicp.ac.cn, E-mail: zhangdh@dicp.ac.cn

2016-03-14

Understanding the role of reactant ro-vibrational degrees of freedom (DOFs) in reaction dynamics of polyatomic molecular dissociation on metal surfaces is of great importance to explore the complex chemical reaction mechanism. Here, we present an expensive quantum dynamics study of the dissociative chemisorption of CH{sub 4} on a rigid Ni(111) surface by developing an accurate nine-dimensional quantum dynamical model including the DOF of azimuth. Based on a highly accurate fifteen-dimensional potential energy surface built from first principles, our simulations elucidate that the dissociation probability of CH{sub 4} has the strong dependence on azimuth and surface impact site. Some improvements aremore » suggested to obtain the accurate dissociation probability from quantum dynamics simulations.« less

WavePacket: A Matlab package for numerical quantum dynamics.II: Open quantum systems, optimal control, and model reduction

NASA Astrophysics Data System (ADS)

Schmidt, Burkhard; Hartmann, Carsten

2018-07-01

WavePacket is an open-source program package for numeric simulations in quantum dynamics. It can solve time-independent or time-dependent linear Schrödinger and Liouville-von Neumann-equations in one or more dimensions. Also coupled equations can be treated, which allows, e.g., to simulate molecular quantum dynamics beyond the Born-Oppenheimer approximation. Optionally accounting for the interaction with external electric fields within the semi-classical dipole approximation, WavePacket can be used to simulate experiments involving tailored light pulses in photo-induced physics or chemistry. Being highly versatile and offering visualization of quantum dynamics 'on the fly', WavePacket is well suited for teaching or research projects in atomic, molecular and optical physics as well as in physical or theoretical chemistry. Building on the previous Part I [Comp. Phys. Comm. 213, 223-234 (2017)] which dealt with closed quantum systems and discrete variable representations, the present Part II focuses on the dynamics of open quantum systems, with Lindblad operators modeling dissipation and dephasing. This part also describes the WavePacket function for optimal control of quantum dynamics, building on rapid monotonically convergent iteration methods. Furthermore, two different approaches to dimension reduction implemented in WavePacket are documented here. In the first one, a balancing transformation based on the concepts of controllability and observability Gramians is used to identify states that are neither well controllable nor well observable. Those states are either truncated or averaged out. In the other approach, the H2-error for a given reduced dimensionality is minimized by H2 optimal model reduction techniques, utilizing a bilinear iterative rational Krylov algorithm. The present work describes the MATLAB version of WavePacket 5.3.0 which is hosted and further developed at the Sourceforge platform, where also extensive Wiki-documentation as well as numerous worked-out demonstration examples with animated graphics can be found.

Quantum dynamical simulation of photoinduced electron transfer processes in dye-semiconductor systems: theory and application to coumarin 343 at TiO₂.

PubMed

Li, Jingrui; Kondov, Ivan; Wang, Haobin; Thoss, Michael

2015-04-10

A recently developed methodology to simulate photoinduced electron transfer processes at dye-semiconductor interfaces is outlined. The methodology employs a first-principles-based model Hamiltonian and accurate quantum dynamics simulations using the multilayer multiconfiguration time-dependent Hartree approach. This method is applied to study electron injection in the dye-semiconductor system coumarin 343-TiO2. Specifically, the influence of electronic-vibrational coupling is analyzed. Extending previous work, we consider the influence of Dushinsky rotation of the normal modes as well as anharmonicities of the potential energy surfaces on the electron transfer dynamics.

Hybrid annealing: Coupling a quantum simulator to a classical computer

NASA Astrophysics Data System (ADS)

Graß, Tobias; Lewenstein, Maciej

2017-05-01

Finding the global minimum in a rugged potential landscape is a computationally hard task, often equivalent to relevant optimization problems. Annealing strategies, either classical or quantum, explore the configuration space by evolving the system under the influence of thermal or quantum fluctuations. The thermal annealing dynamics can rapidly freeze the system into a low-energy configuration, and it can be simulated well on a classical computer, but it easily gets stuck in local minima. Quantum annealing, on the other hand, can be guaranteed to find the true ground state and can be implemented in modern quantum simulators; however, quantum adiabatic schemes become prohibitively slow in the presence of quasidegeneracies. Here, we propose a strategy which combines ideas from simulated annealing and quantum annealing. In such a hybrid algorithm, the outcome of a quantum simulator is processed on a classical device. While the quantum simulator explores the configuration space by repeatedly applying quantum fluctuations and performing projective measurements, the classical computer evaluates each configuration and enforces a lowering of the energy. We have simulated this algorithm for small instances of the random energy model, showing that it potentially outperforms both simulated thermal annealing and adiabatic quantum annealing. It becomes most efficient for problems involving many quasidegenerate ground states.

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

PubMed

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

2017-07-21

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

Dynamical quantum phase transitions: a review

NASA Astrophysics Data System (ADS)

Heyl, Markus

2018-05-01

Quantum theory provides an extensive framework for the description of the equilibrium properties of quantum matter. Yet experiments in quantum simulators have now opened up a route towards the generation of quantum states beyond this equilibrium paradigm. While these states promise to show properties not constrained by equilibrium principles, such as the equal a priori probability of the microcanonical ensemble, identifying the general properties of nonequilibrium quantum dynamics remains a major challenge, especially in view of the lack of conventional concepts such as free energies. The theory of dynamical quantum phase transitions attempts to identify such general principles by lifting the concept of phase transitions to coherent quantum real-time evolution. This review provides a pedagogical introduction to this field. Starting from the general setting of nonequilibrium dynamics in closed quantum many-body systems, we give the definition of dynamical quantum phase transitions as phase transitions in time with physical quantities becoming nonanalytic at critical times. We summarize the achieved theoretical advances as well as the first experimental observations, and furthermore provide an outlook to major open questions as well as future directions of research.

Dynamical quantum phase transitions: a review.

PubMed

Heyl, Markus

2018-05-01

Quantum theory provides an extensive framework for the description of the equilibrium properties of quantum matter. Yet experiments in quantum simulators have now opened up a route towards the generation of quantum states beyond this equilibrium paradigm. While these states promise to show properties not constrained by equilibrium principles, such as the equal a priori probability of the microcanonical ensemble, identifying the general properties of nonequilibrium quantum dynamics remains a major challenge, especially in view of the lack of conventional concepts such as free energies. The theory of dynamical quantum phase transitions attempts to identify such general principles by lifting the concept of phase transitions to coherent quantum real-time evolution. This review provides a pedagogical introduction to this field. Starting from the general setting of nonequilibrium dynamics in closed quantum many-body systems, we give the definition of dynamical quantum phase transitions as phase transitions in time with physical quantities becoming nonanalytic at critical times. We summarize the achieved theoretical advances as well as the first experimental observations, and furthermore provide an outlook to major open questions as well as future directions of research.

Melt-growth dynamics in CdTe crystals

DOE PAGES

Zhou, X. W.; Ward, D. K.; Wong, B. M.; ...

2012-06-01

We use a new, quantum-mechanics-based bond-order potential (BOP) to reveal melt growth dynamics and fine scale defect formation mechanisms in CdTe crystals. Previous molecular dynamics simulations of semiconductors have shown qualitatively incorrect behavior due to the lack of an interatomic potential capable of predicting both crystalline growth and property trends of many transitional structures encountered during the melt → crystal transformation. Here, we demonstrate successful molecular dynamics simulations of melt growth in CdTe using a BOP that significantly improves over other potentials on property trends of different phases. Our simulations result in a detailed understanding of defect formation during themore » melt growth process. Equally important, we show that the new BOP enables defect formation mechanisms to be studied at a scale level comparable to empirical molecular dynamics simulation methods with a fidelity level approaching quantum-mechanical methods.« less

The effect of sampling techniques used in the multiconfigurational Ehrenfest method

NASA Astrophysics Data System (ADS)

Symonds, C.; Kattirtzi, J. A.; Shalashilin, D. V.

2018-05-01

In this paper, we compare and contrast basis set sampling techniques recently developed for use in the ab initio multiple cloning method, a direct dynamics extension to the multiconfigurational Ehrenfest approach, used recently for the quantum simulation of ultrafast photochemistry. We demonstrate that simultaneous use of basis set cloning and basis function trains can produce results which are converged to the exact quantum result. To demonstrate this, we employ these sampling methods in simulations of quantum dynamics in the spin boson model with a broad range of parameters and compare the results to accurate benchmarks.

The effect of sampling techniques used in the multiconfigurational Ehrenfest method.

PubMed

Symonds, C; Kattirtzi, J A; Shalashilin, D V

2018-05-14

In this paper, we compare and contrast basis set sampling techniques recently developed for use in the ab initio multiple cloning method, a direct dynamics extension to the multiconfigurational Ehrenfest approach, used recently for the quantum simulation of ultrafast photochemistry. We demonstrate that simultaneous use of basis set cloning and basis function trains can produce results which are converged to the exact quantum result. To demonstrate this, we employ these sampling methods in simulations of quantum dynamics in the spin boson model with a broad range of parameters and compare the results to accurate benchmarks.

Coherent quantum dynamics launched by incoherent relaxation in a quantum circuit simulator of a light-harvesting complex

NASA Astrophysics Data System (ADS)

Chin, A. W.; Mangaud, E.; Atabek, O.; Desouter-Lecomte, M.

2018-06-01

Engineering and harnessing coherent excitonic transport in organic nanostructures has recently been suggested as a promising way towards improving manmade light-harvesting materials. However, realizing and testing the dissipative system-environment models underlying these proposals is presently very challenging in supramolecular materials. A promising alternative is to use simpler and highly tunable "quantum simulators" built from programmable qubits, as recently achieved in a superconducting circuit by Potočnik et al. [A. Potočnik et al., Nat. Commun. 9, 904 (2018), 10.1038/s41467-018-03312-x]. We simulate the real-time dynamics of an exciton coupled to a quantum bath as it moves through a network based on the quantum circuit of Potočnik et al. Using the numerically exact hierarchical equations of motion to capture the open quantum system dynamics, we find that an ultrafast but completely incoherent relaxation from a high-lying "bright" exciton into a doublet of closely spaced "dark" excitons can spontaneously generate electronic coherences and oscillatory real-space motion across the network (quantum beats). Importantly, we show that this behavior also survives when the environmental noise is classically stochastic (effectively high temperature), as in present experiments. These predictions highlight the possibilities of designing matched electronic and spectral noise structures for robust coherence generation that do not require coherent excitation or cold environments.

Efficient prediction of terahertz quantum cascade laser dynamics from steady-state simulations

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

Agnew, G.; Lim, Y. L.; Nikolić, M.

2015-04-20

Terahertz-frequency quantum cascade lasers (THz QCLs) based on bound-to-continuum active regions are difficult to model owing to their large number of quantum states. We present a computationally efficient reduced rate equation (RE) model that reproduces the experimentally observed variation of THz power with respect to drive current and heat-sink temperature. We also present dynamic (time-domain) simulations under a range of drive currents and predict an increase in modulation bandwidth as the current approaches the peak of the light–current curve, as observed experimentally in mid-infrared QCLs. We account for temperature and bias dependence of the carrier lifetimes, gain, and injection efficiency,more » calculated from a full rate equation model. The temperature dependence of the simulated threshold current, emitted power, and cut-off current are thus all reproduced accurately with only one fitting parameter, the interface roughness, in the full REs. We propose that the model could therefore be used for rapid dynamical simulation of QCL designs.« less

Automated chemical kinetic modeling via hybrid reactive molecular dynamics and quantum chemistry simulations.

PubMed

Döntgen, Malte; Schmalz, Felix; Kopp, Wassja A; Kröger, Leif C; Leonhard, Kai

2018-06-13

An automated scheme for obtaining chemical kinetic models from scratch using reactive molecular dynamics and quantum chemistry simulations is presented. This methodology combines the phase space sampling of reactive molecular dynamics with the thermochemistry and kinetics prediction capabilities of quantum mechanics. This scheme provides the NASA polynomial and modified Arrhenius equation parameters for all species and reactions that are observed during the simulation and supplies them in the ChemKin format. The ab initio level of theory for predictions is easily exchangeable and the presently used G3MP2 level of theory is found to reliably reproduce hydrogen and methane oxidation thermochemistry and kinetics data. Chemical kinetic models obtained with this approach are ready-to-use for, e.g., ignition delay time simulations, as shown for hydrogen combustion. The presented extension of the ChemTraYzer approach can be used as a basis for methodologically advancing chemical kinetic modeling schemes and as a black-box approach to generate chemical kinetic models.

Conformational Dynamics Guides Coherent Exciton Migration in Conjugated Polymer Materials: First-Principles Quantum Dynamical Study

NASA Astrophysics Data System (ADS)

Binder, Robert; Lauvergnat, David; Burghardt, Irene

2018-06-01

We report on high-dimensional quantum dynamical simulations of photoinduced exciton migration in a single-chain oligothiophene segment, in view of elucidating the controversial nature of the elementary exciton transport steps in semiconducting polymers. A novel first-principles parametrized Frenkel J aggregate Hamiltonian is employed that goes significantly beyond the standard Frenkel-Holstein Hamiltonian. Departing from a nonequilibrium state created by photoexcitation, these simulations provide evidence of an ultrafast two-timescale process at low temperatures, involving exciton-polaron formation within tens of femtoseconds (fs), followed by torsional relaxation on an ˜400 fs timescale. The second step is the driving force for exciton migration, as initial conjugation breaks are removed by dynamical planarization. The quantum coherent nature of the elementary exciton migration step is consistent with experimental observations highlighting the correlated and vibrationally coherent nature of the dynamics on ultrafast timescales.

Conformational Dynamics Guides Coherent Exciton Migration in Conjugated Polymer Materials: First-Principles Quantum Dynamical Study.

PubMed

Binder, Robert; Lauvergnat, David; Burghardt, Irene

2018-06-01

We report on high-dimensional quantum dynamical simulations of photoinduced exciton migration in a single-chain oligothiophene segment, in view of elucidating the controversial nature of the elementary exciton transport steps in semiconducting polymers. A novel first-principles parametrized Frenkel J aggregate Hamiltonian is employed that goes significantly beyond the standard Frenkel-Holstein Hamiltonian. Departing from a nonequilibrium state created by photoexcitation, these simulations provide evidence of an ultrafast two-timescale process at low temperatures, involving exciton-polaron formation within tens of femtoseconds (fs), followed by torsional relaxation on an ∼400  fs timescale. The second step is the driving force for exciton migration, as initial conjugation breaks are removed by dynamical planarization. The quantum coherent nature of the elementary exciton migration step is consistent with experimental observations highlighting the correlated and vibrationally coherent nature of the dynamics on ultrafast timescales.

A 2D Array of 100's of Ions for Quantum Simulation and Many-Body Physics in a Penning Trap

NASA Astrophysics Data System (ADS)

Bohnet, Justin; Sawyer, Brian; Britton, Joseph; Bollinger, John

2015-05-01

Quantum simulations promise to reveal new materials and phenomena for experimental study, but few systems have demonstrated the capability to control ensembles in which quantum effects cannot be directly computed. One possible platform for intractable quantum simulations may be a system of 100's of 9Be+ ions in a Penning trap, where the valence electron spins are coupled with an effective Ising interaction in a 2D geometry. Here we report on results from a new Penning trap designed for 2D quantum simulations. We characterize the ion crystal stability and describe progress towards bench-marking quantum effects of the spin-spin coupling using a spin-squeezing witness. We also report on the successful photodissociation of BeH+ contaminant molecular ions that impede the use of such crystals for quantum simulation. This work lays the foundation for future experiments such as the observation of spin dynamics under the quantum Ising Hamiltonian with a transverse field. Supported by a NIST-NRC Research Associateship.

A Study on Fast Gates for Large-Scale Quantum Simulation with Trapped Ions

PubMed Central

Taylor, Richard L.; Bentley, Christopher D. B.; Pedernales, Julen S.; Lamata, Lucas; Solano, Enrique; Carvalho, André R. R.; Hope, Joseph J.

2017-01-01

Large-scale digital quantum simulations require thousands of fundamental entangling gates to construct the simulated dynamics. Despite success in a variety of small-scale simulations, quantum information processing platforms have hitherto failed to demonstrate the combination of precise control and scalability required to systematically outmatch classical simulators. We analyse how fast gates could enable trapped-ion quantum processors to achieve the requisite scalability to outperform classical computers without error correction. We analyze the performance of a large-scale digital simulator, and find that fidelity of around 70% is realizable for π-pulse infidelities below 10−5 in traps subject to realistic rates of heating and dephasing. This scalability relies on fast gates: entangling gates faster than the trap period. PMID:28401945

A Study on Fast Gates for Large-Scale Quantum Simulation with Trapped Ions.

PubMed

Taylor, Richard L; Bentley, Christopher D B; Pedernales, Julen S; Lamata, Lucas; Solano, Enrique; Carvalho, André R R; Hope, Joseph J

2017-04-12

Large-scale digital quantum simulations require thousands of fundamental entangling gates to construct the simulated dynamics. Despite success in a variety of small-scale simulations, quantum information processing platforms have hitherto failed to demonstrate the combination of precise control and scalability required to systematically outmatch classical simulators. We analyse how fast gates could enable trapped-ion quantum processors to achieve the requisite scalability to outperform classical computers without error correction. We analyze the performance of a large-scale digital simulator, and find that fidelity of around 70% is realizable for π-pulse infidelities below 10 -5 in traps subject to realistic rates of heating and dephasing. This scalability relies on fast gates: entangling gates faster than the trap period.

Mixed quantum-classical simulations of the vibrational relaxation of photolyzed carbon monoxide in a hemoprotein

NASA Astrophysics Data System (ADS)

Schubert, Alexander; Falvo, Cyril; Meier, Christoph

2016-08-01

We present mixed quantum-classical simulations on relaxation and dephasing of vibrationally excited carbon monoxide within a protein environment. The methodology is based on a vibrational surface hopping approach treating the vibrational states of CO quantum mechanically, while all remaining degrees of freedom are described by means of classical molecular dynamics. The CO vibrational states form the "surfaces" for the classical trajectories of protein and solvent atoms. In return, environmentally induced non-adiabatic couplings between these states cause transitions describing the vibrational relaxation from first principles. The molecular dynamics simulation yields a detailed atomistic picture of the energy relaxation pathways, taking the molecular structure and dynamics of the protein and its solvent fully into account. Using the ultrafast photolysis of CO in the hemoprotein FixL as an example, we study the relaxation of vibrationally excited CO and evaluate the role of each of the FixL residues forming the heme pocket.

Communication: Quantum molecular dynamics simulation of liquid para-hydrogen by nuclear and electron wave packet approach

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

Hyeon-Deuk, Kim, E-mail: kim@kuchem.kyoto-u.ac.jp; Japan Science and Technology Agency, PRESTO, 4-1-8 Honcho, Kawaguchi, Saitama 332-0012; Ando, Koji

2014-05-07

Liquid para-hydrogen (p-H{sub 2}) is a typical quantum liquid which exhibits strong nuclear quantum effects (NQEs) and thus anomalous static and dynamic properties. We propose a real-time simulation method of wave packet (WP) molecular dynamics (MD) based on non-empirical intra- and inter-molecular interactions of non-spherical hydrogen molecules, and apply it to condensed-phase p-H{sub 2}. The NQEs, such as WP delocalization and zero-point energy, are taken into account without perturbative expansion of prepared model potential functions but with explicit interactions between nuclear and electron WPs. The developed MD simulation for 100 ps with 1200 hydrogen molecules is realized at feasible computationalmore » cost, by which basic experimental properties of p-H{sub 2} liquid such as radial distribution functions, self-diffusion coefficients, and shear viscosities are all well reproduced.« less

Quantum Molecular Dynamics Simulations of Nanotube Tip Assisted Reactions

NASA Technical Reports Server (NTRS)

Menon, Madhu

1998-01-01

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

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.

Atomic quantum simulation of the lattice gauge-Higgs model: Higgs couplings and emergence of exact local gauge symmetry.

PubMed

Kasamatsu, Kenichi; Ichinose, Ikuo; Matsui, Tetsuo

2013-09-13

Recently, the possibility of quantum simulation of dynamical gauge fields was pointed out by using a system of cold atoms trapped on each link in an optical lattice. However, to implement exact local gauge invariance, fine-tuning the interaction parameters among atoms is necessary. In the present Letter, we study the effect of violation of the U(1) local gauge invariance by relaxing the fine-tuning of the parameters and showing that a wide variety of cold atoms is still a faithful quantum simulator for a U(1) gauge-Higgs model containing a Higgs field sitting on sites. The clarification of the dynamics of this gauge-Higgs model sheds some light upon various unsolved problems, including the inflation process of the early Universe. We study the phase structure of this model by Monte Carlo simulation and also discuss the atomic characteristics of the Higgs phase in each simulator.

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.

Simulation of wave packet tunneling of interacting identical particles

NASA Astrophysics Data System (ADS)

Lozovik, Yu. E.; Filinov, A. V.; Arkhipov, A. S.

2003-02-01

We demonstrate a different method of simulation of nonstationary quantum processes, considering the tunneling of two interacting identical particles, represented by wave packets. The used method of quantum molecular dynamics (WMD) is based on the Wigner representation of quantum mechanics. In the context of this method ensembles of classical trajectories are used to solve quantum Wigner-Liouville equation. These classical trajectories obey Hamiltonian-like equations, where the effective potential consists of the usual classical term and the quantum term, which depends on the Wigner function and its derivatives. The quantum term is calculated using local distribution of trajectories in phase space, therefore, classical trajectories are not independent, contrary to classical molecular dynamics. The developed WMD method takes into account the influence of exchange and interaction between particles. The role of direct and exchange interactions in tunneling is analyzed. The tunneling times for interacting particles are calculated.

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.

Emergence of coherence and the dynamics of quantum phase transitions

PubMed Central

Braun, Simon; Friesdorf, Mathis; Hodgman, Sean S.; Schreiber, Michael; Ronzheimer, Jens Philipp; Riera, Arnau; del Rey, Marco; Bloch, Immanuel; Eisert, Jens

2015-01-01

The dynamics of quantum phase transitions pose one of the most challenging problems in modern many-body physics. Here, we study a prototypical example in a clean and well-controlled ultracold atom setup by observing the emergence of coherence when crossing the Mott insulator to superfluid quantum phase transition. In the 1D Bose–Hubbard model, we find perfect agreement between experimental observations and numerical simulations for the resulting coherence length. We, thereby, perform a largely certified analog quantum simulation of this strongly correlated system reaching beyond the regime of free quasiparticles. Experimentally, we additionally explore the emergence of coherence in higher dimensions, where no classical simulations are available, as well as for negative temperatures. For intermediate quench velocities, we observe a power-law behavior of the coherence length, reminiscent of the Kibble–Zurek mechanism. However, we find nonuniversal exponents that cannot be captured by this mechanism or any other known model. PMID:25775515

Towards Quantum Simulation with Circular Rydberg Atoms

NASA Astrophysics Data System (ADS)

Nguyen, T. L.; Raimond, J. M.; Sayrin, C.; Cortiñas, R.; Cantat-Moltrecht, T.; Assemat, F.; Dotsenko, I.; Gleyzes, S.; Haroche, S.; Roux, G.; Jolicoeur, Th.; Brune, M.

2018-01-01

The main objective of quantum simulation is an in-depth understanding of many-body physics, which is important for fundamental issues (quantum phase transitions, transport, …) and for the development of innovative materials. Analytic approaches to many-body systems are limited, and the huge size of their Hilbert space makes numerical simulations on classical computers intractable. A quantum simulator avoids these limitations by transcribing the system of interest into another, with the same dynamics but with interaction parameters under control and with experimental access to all relevant observables. Quantum simulation of spin systems is being explored with trapped ions, neutral atoms, and superconducting devices. We propose here a new paradigm for quantum simulation of spin-1 /2 arrays, providing unprecedented flexibility and allowing one to explore domains beyond the reach of other platforms. It is based on laser-trapped circular Rydberg atoms. Their long intrinsic lifetimes, combined with the inhibition of their microwave spontaneous emission and their low sensitivity to collisions and photoionization, make trapping lifetimes in the minute range realistic with state-of-the-art techniques. Ultracold defect-free circular atom chains can be prepared by a variant of the evaporative cooling method. This method also leads to the detection of arbitrary spin observables with single-site resolution. The proposed simulator realizes an X X Z spin-1 /2 Hamiltonian with nearest-neighbor couplings ranging from a few to tens of kilohertz. All the model parameters can be dynamically tuned at will, making a large range of simulations accessible. The system evolution can be followed over times in the range of seconds, long enough to be relevant for ground-state adiabatic preparation and for the study of thermalization, disorder, or Floquet time crystals. The proposed platform already presents unrivaled features for quantum simulation of regular spin chains. We discuss extensions towards more general quantum simulations of interacting spin systems with full control on individual interactions.

Synthesis, Characterization, and Multimillion-Atom Simulation of Halogen-Based Energetic Materials for Agent Defeat

DTIC Science & Technology

2013-04-01

DTRA-TR-13-23 Synthesis, Characterization, and Multimillion -Atom Simulation of Halogen-Based Energetic Materials for Agent Defeat Approved for...reagents for the destruction of biologically active materials and a simulation of their reactions on a multimillion atom scale with quantum...explosives for destruction of chemical & biological agents. Multimillion -atom molecular dynamics simulations with quantum mechanical accuracy were

Thermal dynamics on the lattice with exponentially improved accuracy

NASA Astrophysics Data System (ADS)

Pawlowski, Jan M.; Rothkopf, Alexander

2018-03-01

We present a novel simulation prescription for thermal quantum fields on a lattice that operates directly in imaginary frequency space. By distinguishing initial conditions from quantum dynamics it provides access to correlation functions also outside of the conventional Matsubara frequencies ωn = 2 πnT. In particular it resolves their frequency dependence between ω = 0 and ω1 = 2 πT, where the thermal physics ω ∼ T of e.g. transport phenomena is dominantly encoded. Real-time spectral functions are related to these correlators via an integral transform with rational kernel, so that their unfolding from the novel simulation data is exponentially improved compared to standard Euclidean simulations. We demonstrate this improvement within a non-trivial 0 + 1-dimensional quantum mechanical toy-model and show that spectral features inaccessible in standard Euclidean simulations are quantitatively captured.

Massive quantum regions for simulations on bio-nanomaterials: synthetic ferritin nanocages.

PubMed

Torras, Juan; Alemán, Carlos

2018-02-22

QM/MM molecular dynamics simulations on the 4His-ΔC* protein cage have been performed using multiple active zones (up to 86 quantum regions). The regulation and nanocage stability exerted by the divalent transition metal ions in the monomer-to-cage conversion have been understood by comparing high level quantum trajectories obtained using Cu 2+ and Ni 2+ coordination ions.

Time reversal and charge conjugation in an embedding quantum simulator.

PubMed

Zhang, Xiang; Shen, Yangchao; Zhang, Junhua; Casanova, Jorge; Lamata, Lucas; Solano, Enrique; Yung, Man-Hong; Zhang, Jing-Ning; Kim, Kihwan

2015-08-04

A quantum simulator is an important device that may soon outperform current classical computations. A basic arithmetic operation, the complex conjugate, however, is considered to be impossible to be implemented in such a quantum system due to the linear character of quantum mechanics. Here, we present the experimental quantum simulation of such an unphysical operation beyond the regime of unitary and dissipative evolutions through the embedding of a quantum dynamics in the electronic multilevels of a (171)Yb(+) ion. We perform time reversal and charge conjugation, which are paradigmatic examples of antiunitary symmetry operators, in the evolution of a Majorana equation without the tomographic knowledge of the evolving state. Thus, these operations can be applied regardless of the system size. Our approach offers the possibility to add unphysical operations to the toolbox of quantum simulation, and provides a route to efficiently compute otherwise intractable quantities, such as entanglement monotones.

Time reversal and charge conjugation in an embedding quantum simulator

PubMed Central

Zhang, Xiang; Shen, Yangchao; Zhang, Junhua; Casanova, Jorge; Lamata, Lucas; Solano, Enrique; Yung, Man-Hong; Zhang, Jing-Ning; Kim, Kihwan

2015-01-01

A quantum simulator is an important device that may soon outperform current classical computations. A basic arithmetic operation, the complex conjugate, however, is considered to be impossible to be implemented in such a quantum system due to the linear character of quantum mechanics. Here, we present the experimental quantum simulation of such an unphysical operation beyond the regime of unitary and dissipative evolutions through the embedding of a quantum dynamics in the electronic multilevels of a 171Yb+ ion. We perform time reversal and charge conjugation, which are paradigmatic examples of antiunitary symmetry operators, in the evolution of a Majorana equation without the tomographic knowledge of the evolving state. Thus, these operations can be applied regardless of the system size. Our approach offers the possibility to add unphysical operations to the toolbox of quantum simulation, and provides a route to efficiently compute otherwise intractable quantities, such as entanglement monotones. PMID:26239028

A simulator for discrete quantum walks on lattices

NASA Astrophysics Data System (ADS)

Rodrigues, J.; Paunković, N.; Mateus, P.

In this paper, we present a simulator for two-particle quantum walks on the line and one-particle on a two-dimensional squared lattice. It can be used to investigate the equivalence between the two cases (one- and two-particle walks) for various boundary conditions (open, circular, reflecting, absorbing and their combinations). For the case of a single walker on a two-dimensional lattice, the simulator can also implement the Möbius strip. Furthermore, other topologies for the walker are also simulated by the proposed tool, like certain types of planar graphs with degree up to 4, by considering missing links over the lattice. The main purpose of the simulator is to study the genuinely quantum effects on the global properties of the two-particle joint probability distribution on the entanglement between the walkers/axis. For that purpose, the simulator is designed to compute various quantities such as: the entanglement and classical correlations, (classical and quantum) mutual information, the average distance between the two walkers, different hitting times and quantum discord. These quantities are of vital importance in designing possible algorithmic applications of quantum walks, namely in search, 3-SAT problems, etc. The simulator can also implement the static partial measurements of particle(s) positions and dynamic breaking of the links between certain nodes, both of which can be used to investigate the effects of decoherence on the walker(s). Finally, the simulator can be used to investigate the dynamic Anderson-like particle localization by varying the coin operators of certain nodes on the line/lattice. We also present some illustrative and relevant examples of one- and two-particle quantum walks in various scenarios. The tool was implemented in C and is available on-line at http://qwsim.weebly.com/.

Real-time dynamics of lattice gauge theories with a few-qubit quantum computer

NASA Astrophysics Data System (ADS)

Martinez, Esteban A.; Muschik, Christine A.; Schindler, Philipp; Nigg, Daniel; Erhard, Alexander; Heyl, Markus; Hauke, Philipp; Dalmonte, Marcello; Monz, Thomas; Zoller, Peter; Blatt, Rainer

2016-06-01

Gauge theories are fundamental to our understanding of interactions between the elementary constituents of matter as mediated by gauge bosons. However, computing the real-time dynamics in gauge theories is a notorious challenge for classical computational methods. This has recently stimulated theoretical effort, using Feynman’s idea of a quantum simulator, to devise schemes for simulating such theories on engineered quantum-mechanical devices, with the difficulty that gauge invariance and the associated local conservation laws (Gauss laws) need to be implemented. Here we report the experimental demonstration of a digital quantum simulation of a lattice gauge theory, by realizing (1 + 1)-dimensional quantum electrodynamics (the Schwinger model) on a few-qubit trapped-ion quantum computer. We are interested in the real-time evolution of the Schwinger mechanism, describing the instability of the bare vacuum due to quantum fluctuations, which manifests itself in the spontaneous creation of electron-positron pairs. To make efficient use of our quantum resources, we map the original problem to a spin model by eliminating the gauge fields in favour of exotic long-range interactions, which can be directly and efficiently implemented on an ion trap architecture. We explore the Schwinger mechanism of particle-antiparticle generation by monitoring the mass production and the vacuum persistence amplitude. Moreover, we track the real-time evolution of entanglement in the system, which illustrates how particle creation and entanglement generation are directly related. Our work represents a first step towards quantum simulation of high-energy theories using atomic physics experiments—the long-term intention is to extend this approach to real-time quantum simulations of non-Abelian lattice gauge theories.

Zero-Point Energy Constraint for Unimolecular Dissociation Reactions. Giving Trajectories Multiple Chances To Dissociate Correctly.

PubMed

Paul, Amit K; Hase, William L

2016-01-28

A zero-point energy (ZPE) constraint model is proposed for classical trajectory simulations of unimolecular decomposition and applied to CH4* → H + CH3 decomposition. With this model trajectories are not allowed to dissociate unless they have ZPE in the CH3 product. If not, they are returned to the CH4* region of phase space and, if necessary, given additional opportunities to dissociate with ZPE. The lifetime for dissociation of an individual trajectory is the time it takes to dissociate with ZPE in CH3, including multiple possible returns to CH4*. With this ZPE constraint the dissociation of CH4* is exponential in time as expected for intrinsic RRKM dynamics and the resulting rate constant is in good agreement with the harmonic quantum value of RRKM theory. In contrast, a model that discards trajectories without ZPE in the reaction products gives a CH4* → H + CH3 rate constant that agrees with the classical and not quantum RRKM value. The rate constant for the purely classical simulation indicates that anharmonicity may be important and the rate constant from the ZPE constrained classical trajectory simulation may not represent the complete anharmonicity of the RRKM quantum dynamics. The ZPE constraint model proposed here is compared with previous models for restricting ZPE flow in intramolecular dynamics, and connecting product and reactant/product quantum energy levels in chemical dynamics simulations.

Computer studies of multiple-quantum spin dynamics

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

Murdoch, J.B.

The excitation and detection of multiple-quantum (MQ) transitions in Fourier transform NMR spectroscopy is an interesting problem in the quantum mechanical dynamics of spin systems as well as an important new technique for investigation of molecular structure. In particular, multiple-quantum spectroscopy can be used to simplify overly complex spectra or to separate the various interactions between a nucleus and its environment. The emphasis of this work is on computer simulation of spin-system evolution to better relate theory and experiment.

Ab Initio Path Integral Molecular Dynamics Study of the Nuclear Quantum Effect on Out-of-Plane Ring Deformation of Hydrogen Maleate Anion.

PubMed

Kawashima, Yukio; Tachikawa, Masanori

2014-01-14

Ab initio path integral molecular dynamics (PIMD) simulation was performed to understand the nuclear quantum effect on the out-of-plane ring deformation of hydrogen maleate anion and investigate the existence of a stable structure with ring deformation, which was suggested in experimental observation (Fillaux et al., Chem. Phys. 1999, 120, 387-403). The isotope effect and the temperature effect are studied as well. We first investigated the nuclear quantum effect on the proton transfer. In static calculation and classical ab initio molecular dynamics simulations, the proton in the hydrogen bond is localized to either oxygen atom. On the other hand, the proton is located at the center of two oxygen atoms in quantum ab initio PIMD simulations. The nuclear quantum effect washes out the barrier of proton transfer. We next examined the nuclear quantum effect on the motion of hydrogen maleate anion. Principal component analysis revealed that the out-of-plane ring bending modes have dominant contribution to the entire molecular motion. In quantum ab initio PIMD simulations, structures with ring deformation were the global minimum for the deuterated isotope at 300 K. We analyzed the out-of-plane ring bending mode further and found that there are three minima along a ring distortion mode. We successfully found a stable structure with ring deformation of hydrogen maleate for the first time, to our knowledge, using theoretical calculation. The structures with ring deformation found in quantum simulation of the deuterated isotope allowed the proton transfer to occur more frequently than the planar structure. Static ab initio electronic structure calculation found that the structures with ring deformation have very small proton transfer barrier compared to the planar structure. We suggest that the "proton transfer driven" mechanism is the origin of stabilization for the structure with out-of-plane ring deformation.

Trapping photons on the line: controllable dynamics of a quantum walk

NASA Astrophysics Data System (ADS)

Xue, Peng; Qin, Hao; Tang, Bao

2014-04-01

Optical interferometers comprising birefringent-crystal beam displacers, wave plates, and phase shifters serve as stable devices for simulating quantum information processes such as heralded coined quantum walks. Quantum walks are important for quantum algorithms, universal quantum computing circuits, quantum transport in complex systems, and demonstrating intriguing nonlinear dynamical quantum phenomena. We introduce fully controllable polarization-independent phase shifters in optical pathes in order to realize site-dependent phase defects. The effectiveness of our interferometer is demonstrated through realizing single-photon quantum-walk dynamics in one dimension. By applying site-dependent phase defects, the translational symmetry of an ideal standard quantum walk is broken resulting in localization effect in a quantum walk architecture. The walk is realized for different site-dependent phase defects and coin settings, indicating the strength of localization signature depends on the level of phase due to site-dependent phase defects and coin settings and opening the way for the implementation of a quantum-walk-based algorithm.

QMMMW: A wrapper for QM/MM simulations with QUANTUM ESPRESSO and LAMMPS

NASA Astrophysics Data System (ADS)

Ma, Changru; Martin-Samos, Layla; Fabris, Stefano; Laio, Alessandro; Piccinin, Simone

2015-10-01

We present QMMMW, a new program aimed at performing Quantum Mechanics/Molecular Mechanics (QM/MM) molecular dynamics. The package operates as a wrapper that patches PWscf code included in the QUANTUM ESPRESSO distribution and LAMMPS Molecular Dynamics Simulator. It is designed with a paradigm based on three guidelines: (i) minimal amount of modifications on the parent codes, (ii) flexibility and computational efficiency of the communication layer and (iii) accuracy of the Hamiltonian describing the interaction between the QM and MM subsystems. These three features are seldom present simultaneously in other implementations of QMMM. The QMMMW project is hosted by qe-forge at

Equivalence principle and quantum mechanics: quantum simulation with entangled photons.

PubMed

Longhi, S

2018-01-15

Einstein's equivalence principle (EP) states the complete physical equivalence of a gravitational field and corresponding inertial field in an accelerated reference frame. However, to what extent the EP remains valid in non-relativistic quantum mechanics is a controversial issue. To avoid violation of the EP, Bargmann's superselection rule forbids a coherent superposition of states with different masses. Here we suggest a quantum simulation of non-relativistic Schrödinger particle dynamics in non-inertial reference frames, which is based on the propagation of polarization-entangled photon pairs in curved and birefringent optical waveguides and Hong-Ou-Mandel quantum interference measurement. The photonic simulator can emulate superposition of mass states, which would lead to violation of the EP.

Semiclassical dynamics of spin density waves

NASA Astrophysics Data System (ADS)

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

2018-01-01

We present a theoretical framework for equilibrium and nonequilibrium dynamical simulation of quantum states with spin-density-wave (SDW) order. Within a semiclassical adiabatic approximation that retains electron degrees of freedom, we demonstrate that the SDW order parameter obeys a generalized Landau-Lifshitz equation. With the aid of an enhanced kernel polynomial method, our linear-scaling quantum Landau-Lifshitz dynamics (QLLD) method enables dynamical SDW simulations with N ≃105 lattice sites. Our real-space formulation can be used to compute dynamical responses, such as the dynamical structure factor, of complex and even inhomogeneous SDW configurations at zero or finite temperatures. Applying the QLLD to study the relaxation of a noncoplanar topological SDW under the excitation of a short pulse, we further demonstrate the crucial role of spatial correlations and fluctuations in the SDW dynamics.

Comment on "A centroid molecular dynamics study of liquid para hydrogen and ortho deuterium" [J. Chem. Phys. 121, 6412 (2004)].

PubMed

Miller, Thomas F; Manolopoulos, David E; Madden, Paul A; Konieczny, Martin; Oberhofer, Harald

2005-02-01

We show that the two phase points considered in the recent simulations of liquid para hydrogen by Hone and Voth lie in the liquid-vapor coexistence region of a purely classical molecular dynamics simulation. By contrast, their phase point for ortho deuterium was in the one-phase liquid region for both classical and quantum simulations. These observations are used to account for their report that quantum mechanical effects enhance the diffusion in liquid para hydrogen and decrease it in ortho deuterium.(c) 2005 American Institute of Physics.

An analytical derivation of MC-SCF vibrational wave functions for the quantum dynamical simulation of multiple proton transfer reactions: Initial application to protonated water chains

NASA Astrophysics Data System (ADS)

Drukker, Karen; Hammes-Schiffer, Sharon

1997-07-01

This paper presents an analytical derivation of a multiconfigurational self-consistent-field (MC-SCF) solution of the time-independent Schrödinger equation for nuclear motion (i.e. vibrational modes). This variational MC-SCF method is designed for the mixed quantum/classical molecular dynamics simulation of multiple proton transfer reactions, where the transferring protons are treated quantum mechanically while the remaining degrees of freedom are treated classically. This paper presents a proof that the Hellmann-Feynman forces on the classical degrees of freedom are identical to the exact forces (i.e. the Pulay corrections vanish) when this MC-SCF method is used with an appropriate choice of basis functions. This new MC-SCF method is applied to multiple proton transfer in a protonated chain of three hydrogen-bonded water molecules. The ground state and the first three excited state energies and the ground state forces agree well with full configuration interaction calculations. Sample trajectories are obtained using adiabatic molecular dynamics methods, and nonadiabatic effects are found to be insignificant for these sample trajectories. The accuracy of the excited states will enable this MC-SCF method to be used in conjunction with nonadiabatic molecular dynamics methods. This application differs from previous work in that it is a real-time quantum dynamical nonequilibrium simulation of multiple proton transfer in a chain of water molecules.

MCTDH on-the-fly: Efficient grid-based quantum dynamics without pre-computed potential energy surfaces

NASA Astrophysics Data System (ADS)

Richings, Gareth W.; Habershon, Scott

2018-04-01

We present significant algorithmic improvements to a recently proposed direct quantum dynamics method, based upon combining well established grid-based quantum dynamics approaches and expansions of the potential energy operator in terms of a weighted sum of Gaussian functions. Specifically, using a sum of low-dimensional Gaussian functions to represent the potential energy surface (PES), combined with a secondary fitting of the PES using singular value decomposition, we show how standard grid-based quantum dynamics methods can be dramatically accelerated without loss of accuracy. This is demonstrated by on-the-fly simulations (using both standard grid-based methods and multi-configuration time-dependent Hartree) of both proton transfer on the electronic ground state of salicylaldimine and the non-adiabatic dynamics of pyrazine.

Delayed coherent quantum feedback from a scattering theory and a matrix product state perspective

NASA Astrophysics Data System (ADS)

Guimond, P.-O.; Pletyukhov, M.; Pichler, H.; Zoller, P.

2017-12-01

We study the scattering of photons propagating in a semi-infinite waveguide terminated by a mirror and interacting with a quantum emitter. This paradigm constitutes an example of coherent quantum feedback, where light emitted towards the mirror gets redirected back to the emitter. We derive an analytical solution for the scattering of two-photon states, which is based on an exact resummation of the perturbative expansion of the scattering matrix, in a regime where the time delay of the coherent feedback is comparable to the timescale of the quantum emitter’s dynamics. We compare the results with numerical simulations based on matrix product state techniques simulating the full dynamics of the system, and extend the study to the scattering of coherent states beyond the low-power limit.

Numerical characteristics of quantum computer simulation

NASA Astrophysics Data System (ADS)

Chernyavskiy, A.; Khamitov, K.; Teplov, A.; Voevodin, V.; Voevodin, Vl.

2016-12-01

The simulation of quantum circuits is significantly important for the implementation of quantum information technologies. The main difficulty of such modeling is the exponential growth of dimensionality, thus the usage of modern high-performance parallel computations is relevant. As it is well known, arbitrary quantum computation in circuit model can be done by only single- and two-qubit gates, and we analyze the computational structure and properties of the simulation of such gates. We investigate the fact that the unique properties of quantum nature lead to the computational properties of the considered algorithms: the quantum parallelism make the simulation of quantum gates highly parallel, and on the other hand, quantum entanglement leads to the problem of computational locality during simulation. We use the methodology of the AlgoWiki project (algowiki-project.org) to analyze the algorithm. This methodology consists of theoretical (sequential and parallel complexity, macro structure, and visual informational graph) and experimental (locality and memory access, scalability and more specific dynamic characteristics) parts. Experimental part was made by using the petascale Lomonosov supercomputer (Moscow State University, Russia). We show that the simulation of quantum gates is a good base for the research and testing of the development methods for data intense parallel software, and considered methodology of the analysis can be successfully used for the improvement of the algorithms in quantum information science.

Simulation of Quantum Many-Body Dynamics for Generic Strongly-Interacting Systems

NASA Astrophysics Data System (ADS)

Meyer, Gregory; Machado, Francisco; Yao, Norman

2017-04-01

Recent experimental advances have enabled the bottom-up assembly of complex, strongly interacting quantum many-body systems from individual atoms, ions, molecules and photons. These advances open the door to studying dynamics in isolated quantum systems as well as the possibility of realizing novel out-of-equilibrium phases of matter. Numerical studies provide insight into these systems; however, computational time and memory usage limit common numerical methods such as exact diagonalization to relatively small Hilbert spaces of dimension 215 . Here we present progress toward a new software package for dynamical time evolution of large generic quantum systems on massively parallel computing architectures. By projecting large sparse Hamiltonians into a much smaller Krylov subspace, we are able to compute the evolution of strongly interacting systems with Hilbert space dimension nearing 230. We discuss and benchmark different design implementations, such as matrix-free methods and GPU based calculations, using both pre-thermal time crystals and the Sachdev-Ye-Kitaev model as examples. We also include a simple symbolic language to describe generic Hamiltonians, allowing simulation of diverse quantum systems without any modification of the underlying C and Fortran code.

Tensor-Train Split-Operator Fourier Transform (TT-SOFT) Method: Multidimensional Nonadiabatic Quantum Dynamics.

PubMed

Greene, Samuel M; Batista, Victor S

2017-09-12

We introduce the "tensor-train split-operator Fourier transform" (TT-SOFT) method for simulations of multidimensional nonadiabatic quantum dynamics. TT-SOFT is essentially the grid-based SOFT method implemented in dynamically adaptive tensor-train representations. In the same spirit of all matrix product states, the tensor-train format enables the representation, propagation, and computation of observables of multidimensional wave functions in terms of the grid-based wavepacket tensor components, bypassing the need of actually computing the wave function in its full-rank tensor product grid space. We demonstrate the accuracy and efficiency of the TT-SOFT method as applied to propagation of 24-dimensional wave packets, describing the S 1 /S 2 interconversion dynamics of pyrazine after UV photoexcitation to the S 2 state. Our results show that the TT-SOFT method is a powerful computational approach for simulations of quantum dynamics of polyatomic systems since it avoids the exponential scaling problem of full-rank grid-based representations.

Tree tensor network approach to simulating Shor's algorithm

NASA Astrophysics Data System (ADS)

Dumitrescu, Eugene

2017-12-01

Constructively simulating quantum systems furthers our understanding of qualitative and quantitative features which may be analytically intractable. In this paper, we directly simulate and explore the entanglement structure present in the paradigmatic example for exponential quantum speedups: Shor's algorithm. To perform our simulation, we construct a dynamic tree tensor network which manifestly captures two salient circuit features for modular exponentiation. These are the natural two-register bipartition and the invariance of entanglement with respect to permutations of the top-register qubits. Our construction help identify the entanglement entropy properties, which we summarize by a scaling relation. Further, the tree network is efficiently projected onto a matrix product state from which we efficiently execute the quantum Fourier transform. Future simulation of quantum information states with tensor networks exploiting circuit symmetries is discussed.

Mixed quantum-classical simulations of the vibrational relaxation of photolyzed carbon monoxide in a hemoprotein

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

Schubert, Alexander, E-mail: schubert@irsamc.ups-tlse.fr; Meier, Christoph; Falvo, Cyril

2016-08-07

We present mixed quantum-classical simulations on relaxation and dephasing of vibrationally excited carbon monoxide within a protein environment. The methodology is based on a vibrational surface hopping approach treating the vibrational states of CO quantum mechanically, while all remaining degrees of freedom are described by means of classical molecular dynamics. The CO vibrational states form the “surfaces” for the classical trajectories of protein and solvent atoms. In return, environmentally induced non-adiabatic couplings between these states cause transitions describing the vibrational relaxation from first principles. The molecular dynamics simulation yields a detailed atomistic picture of the energy relaxation pathways, taking themore » molecular structure and dynamics of the protein and its solvent fully into account. Using the ultrafast photolysis of CO in the hemoprotein FixL as an example, we study the relaxation of vibrationally excited CO and evaluate the role of each of the FixL residues forming the heme pocket.« less

Recent Advances and Perspectives on Nonadiabatic Mixed Quantum-Classical Dynamics.

PubMed

Crespo-Otero, Rachel; Barbatti, Mario

2018-05-16

Nonadiabatic mixed quantum-classical (NA-MQC) dynamics methods form a class of computational theoretical approaches in quantum chemistry tailored to investigate the time evolution of nonadiabatic phenomena in molecules and supramolecular assemblies. NA-MQC is characterized by a partition of the molecular system into two subsystems: one to be treated quantum mechanically (usually but not restricted to electrons) and another to be dealt with classically (nuclei). The two subsystems are connected through nonadiabatic couplings terms to enforce self-consistency. A local approximation underlies the classical subsystem, implying that direct dynamics can be simulated, without needing precomputed potential energy surfaces. The NA-MQC split allows reducing computational costs, enabling the treatment of realistic molecular systems in diverse fields. Starting from the three most well-established methods-mean-field Ehrenfest, trajectory surface hopping, and multiple spawning-this review focuses on the NA-MQC dynamics methods and programs developed in the last 10 years. It stresses the relations between approaches and their domains of application. The electronic structure methods most commonly used together with NA-MQC dynamics are reviewed as well. The accuracy and precision of NA-MQC simulations are critically discussed, and general guidelines to choose an adequate method for each application are delivered.

Qubit Architecture with High Coherence and Fast Tunable Coupling.

PubMed

Chen, Yu; Neill, C; Roushan, P; Leung, N; Fang, M; Barends, R; Kelly, J; Campbell, B; Chen, Z; Chiaro, B; Dunsworth, A; Jeffrey, E; Megrant, A; Mutus, J Y; O'Malley, P J J; Quintana, C M; Sank, D; Vainsencher, A; Wenner, J; White, T C; Geller, Michael R; Cleland, A N; Martinis, John M

2014-11-28

We introduce a superconducting qubit architecture that combines high-coherence qubits and tunable qubit-qubit coupling. With the ability to set the coupling to zero, we demonstrate that this architecture is protected from the frequency crowding problems that arise from fixed coupling. More importantly, the coupling can be tuned dynamically with nanosecond resolution, making this architecture a versatile platform with applications ranging from quantum logic gates to quantum simulation. We illustrate the advantages of dynamical coupling by implementing a novel adiabatic controlled-z gate, with a speed approaching that of single-qubit gates. Integrating coherence and scalable control, the introduced qubit architecture provides a promising path towards large-scale quantum computation and simulation.

Scaling analysis and instantons for thermally assisted tunneling and quantum Monte Carlo simulations

NASA Astrophysics Data System (ADS)

Jiang, Zhang; Smelyanskiy, Vadim N.; Isakov, Sergei V.; Boixo, Sergio; Mazzola, Guglielmo; Troyer, Matthias; Neven, Hartmut

2017-01-01

We develop an instantonic calculus to derive an analytical expression for the thermally assisted tunneling decay rate of a metastable state in a fully connected quantum spin model. The tunneling decay problem can be mapped onto the Kramers escape problem of a classical random dynamical field. This dynamical field is simulated efficiently by path-integral quantum Monte Carlo (QMC). We show analytically that the exponential scaling with the number of spins of the thermally assisted quantum tunneling rate and the escape rate of the QMC process are identical. We relate this effect to the existence of a dominant instantonic tunneling path. The instanton trajectory is described by nonlinear dynamical mean-field theory equations for a single-site magnetization vector, which we solve exactly. Finally, we derive scaling relations for the "spiky" barrier shape when the spin tunneling and QMC rates scale polynomially with the number of spins N while a purely classical over-the-barrier activation rate scales exponentially with N .

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

PubMed Central

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

2013-01-01

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

Direct Observation of Dynamical Quantum Phase Transitions in an Interacting Many-Body System

NASA Astrophysics Data System (ADS)

Jurcevic, P.; Shen, H.; Hauke, P.; Maier, C.; Brydges, T.; Hempel, C.; Lanyon, B. P.; Heyl, M.; Blatt, R.; Roos, C. F.

2017-08-01

The theory of phase transitions represents a central concept for the characterization of equilibrium matter. In this work we study experimentally an extension of this theory to the nonequilibrium dynamical regime termed dynamical quantum phase transitions (DQPTs). We investigate and measure DQPTs in a string of ions simulating interacting transverse-field Ising models. During the nonequilibrium dynamics induced by a quantum quench we show for strings of up to 10 ions the direct detection of DQPTs by revealing nonanalytic behavior in time. Moreover, we provide a link between DQPTs and the dynamics of other quantities such as the magnetization, and we establish a connection between DQPTs and entanglement production.

Direct Observation of Dynamical Quantum Phase Transitions in an Interacting Many-Body System.

PubMed

Jurcevic, P; Shen, H; Hauke, P; Maier, C; Brydges, T; Hempel, C; Lanyon, B P; Heyl, M; Blatt, R; Roos, C F

2017-08-25

The theory of phase transitions represents a central concept for the characterization of equilibrium matter. In this work we study experimentally an extension of this theory to the nonequilibrium dynamical regime termed dynamical quantum phase transitions (DQPTs). We investigate and measure DQPTs in a string of ions simulating interacting transverse-field Ising models. During the nonequilibrium dynamics induced by a quantum quench we show for strings of up to 10 ions the direct detection of DQPTs by revealing nonanalytic behavior in time. Moreover, we provide a link between DQPTs and the dynamics of other quantities such as the magnetization, and we establish a connection between DQPTs and entanglement production.

Electron-phonon thermalization in a scalable method for real-time quantum dynamics

NASA Astrophysics Data System (ADS)

Rizzi, Valerio; Todorov, Tchavdar N.; Kohanoff, Jorge J.; Correa, Alfredo A.

2016-01-01

We present a quantum simulation method that follows the dynamics of out-of-equilibrium many-body systems of electrons and oscillators in real time. Its cost is linear in the number of oscillators and it can probe time scales from attoseconds to hundreds of picoseconds. Contrary to Ehrenfest dynamics, it can thermalize starting from a variety of initial conditions, including electronic population inversion. While an electronic temperature can be defined in terms of a nonequilibrium entropy, a Fermi-Dirac distribution in general emerges only after thermalization. These results can be used to construct a kinetic model of electron-phonon equilibration based on the explicit quantum dynamics.

Discrimination of correlated and entangling quantum channels with selective process tomography

DOE PAGES

Dumitrescu, Eugene; Humble, Travis S.

2016-10-10

The accurate and reliable characterization of quantum dynamical processes underlies efforts to validate quantum technologies, where discrimination between competing models of observed behaviors inform efforts to fabricate and operate qubit devices. We present a protocol for quantum channel discrimination that leverages advances in direct characterization of quantum dynamics (DCQD) codes. We demonstrate that DCQD codes enable selective process tomography to improve discrimination between entangling and correlated quantum dynamics. Numerical simulations show selective process tomography requires only a few measurement configurations to achieve a low false alarm rate and that the DCQD encoding improves the resilience of the protocol to hiddenmore » sources of noise. Lastly, our results show that selective process tomography with DCQD codes is useful for efficiently distinguishing sources of correlated crosstalk from uncorrelated noise in current and future experimental platforms.« less

Nonlinear quantum Rabi model in trapped ions

NASA Astrophysics Data System (ADS)

Cheng, Xiao-Hang; Arrazola, Iñigo; Pedernales, Julen S.; Lamata, Lucas; Chen, Xi; Solano, Enrique

2018-02-01

We study the nonlinear dynamics of trapped-ion models far away from the Lamb-Dicke regime. This nonlinearity induces a blockade on the propagation of quantum information along the Hilbert space of the Jaynes-Cummings and quantum Rabi models. We propose to use this blockade as a resource for the dissipative generation of high-number Fock states. Also, we compare the linear and nonlinear cases of the quantum Rabi model in the ultrastrong and deep strong-coupling regimes. Moreover, we propose a scheme to simulate the nonlinear quantum Rabi model in all coupling regimes. This can be done via off-resonant nonlinear red- and blue-sideband interactions in a single trapped ion, yielding applications as a dynamical quantum filter.

Dynamics of open quantum systems by interpolation of von Neumann and classical master equations, and its application to quantum annealing

NASA Astrophysics Data System (ADS)

Kadowaki, Tadashi

2018-02-01

We propose a method to interpolate dynamics of von Neumann and classical master equations with an arbitrary mixing parameter to investigate the thermal effects in quantum dynamics. The two dynamics are mixed by intervening to continuously modify their solutions, thus coupling them indirectly instead of directly introducing a coupling term. This maintains the quantum system in a pure state even after the introduction of thermal effects and obtains not only a density matrix but also a state vector representation. Further, we demonstrate that the dynamics of a two-level system can be rewritten as a set of standard differential equations, resulting in quantum dynamics that includes thermal relaxation. These equations are equivalent to the optical Bloch equations at the weak coupling and asymptotic limits, implying that the dynamics cause thermal effects naturally. Numerical simulations of ferromagnetic and frustrated systems support this idea. Finally, we use this method to study thermal effects in quantum annealing, revealing nontrivial performance improvements for a spin glass model over a certain range of annealing time. This result may enable us to optimize the annealing time of real annealing machines.

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

Dumitrescu, Eugene; Humble, Travis S.

The accurate and reliable characterization of quantum dynamical processes underlies efforts to validate quantum technologies, where discrimination between competing models of observed behaviors inform efforts to fabricate and operate qubit devices. We present a protocol for quantum channel discrimination that leverages advances in direct characterization of quantum dynamics (DCQD) codes. We demonstrate that DCQD codes enable selective process tomography to improve discrimination between entangling and correlated quantum dynamics. Numerical simulations show selective process tomography requires only a few measurement configurations to achieve a low false alarm rate and that the DCQD encoding improves the resilience of the protocol to hiddenmore » sources of noise. Lastly, our results show that selective process tomography with DCQD codes is useful for efficiently distinguishing sources of correlated crosstalk from uncorrelated noise in current and future experimental platforms.« less

Dynamical Casimir Effect for Gaussian Boson Sampling.

PubMed

Peropadre, Borja; Huh, Joonsuk; Sabín, Carlos

2018-02-28

We show that the Dynamical Casimir Effect (DCE), realized on two multimode coplanar waveg-uide resonators, implements a gaussian boson sampler (GBS). The appropriate choice of the mirror acceleration that couples both resonators translates into the desired initial gaussian state and many-boson interference in a boson sampling network. In particular, we show that the proposed quantum simulator naturally performs a classically hard task, known as scattershot boson sampling. Our result unveils an unprecedented computational power of DCE, and paves the way for using DCE as a resource for quantum simulation.

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.

Simulation approach for the evaluation of tracking accuracy in radiotherapy: a preliminary study.

PubMed

Tanaka, Rie; Ichikawa, Katsuhiro; Mori, Shinichiro; Sanada, Sigeru

2013-01-01

Real-time tumor tracking in external radiotherapy can be achieved by diagnostic (kV) X-ray imaging with a dynamic flat-panel detector (FPD). It is important to keep the patient dose as low as possible while maintaining tracking accuracy. A simulation approach would be helpful to optimize the imaging conditions. This study was performed to develop a computer simulation platform based on a noise property of the imaging system for the evaluation of tracking accuracy at any noise level. Flat-field images were obtained using a direct-type dynamic FPD, and noise power spectrum (NPS) analysis was performed. The relationship between incident quantum number and pixel value was addressed, and a conversion function was created. The pixel values were converted into a map of quantum number using the conversion function, and the map was then input into the random number generator to simulate image noise. Simulation images were provided at different noise levels by changing the incident quantum numbers. Subsequently, an implanted marker was tracked automatically and the maximum tracking errors were calculated at different noise levels. The results indicated that the maximum tracking error increased with decreasing incident quantum number in flat-field images with an implanted marker. In addition, the range of errors increased with decreasing incident quantum number. The present method could be used to determine the relationship between image noise and tracking accuracy. The results indicated that the simulation approach would aid in determining exposure dose conditions according to the necessary tracking accuracy.

Fermi resonance in CO2: Mode assignment and quantum nuclear effects from first principles molecular dynamics

NASA Astrophysics Data System (ADS)

Basire, Marie; Mouhat, Félix; Fraux, Guillaume; Bordage, Amélie; Hazemann, Jean-Louis; Louvel, Marion; Spezia, Riccardo; Bonella, Sara; Vuilleumier, Rodolphe

2017-04-01

Vibrational spectroscopy is a fundamental tool to investigate local atomic arrangements and the effect of the environment, provided that the spectral features can be correctly assigned. This can be challenging in experiments and simulations when double peaks are present because they can have different origins. Fermi dyads are a common class of such doublets, stemming from the resonance of the fundamental excitation of a mode with the overtone of another. We present a new, efficient approach to unambiguously characterize Fermi resonances in density functional theory (DFT) based simulations of condensed phase systems. With it, the spectral features can be assigned and the two resonating modes identified. We also show how data from DFT simulations employing classical nuclear dynamics can be post-processed and combined with a perturbative quantum treatment at a finite temperature to include analytically thermal quantum nuclear effects. The inclusion of these effects is crucial to correct some of the qualitative failures of the Newtonian dynamics simulations at a low temperature such as, in particular, the behavior of the frequency splitting of the Fermi dyad. We show, by comparing with experimental data for the paradigmatic case of supercritical CO2, that these thermal quantum effects can be substantial even at ambient conditions and that our scheme provides an accurate and computationally convenient approach to account for them.

Quantum molecular dynamics simulation of structural and thermodynamic properties of NiAl

NASA Astrophysics Data System (ADS)

Karchevskaya, E. S.; Minakov, D. V.; Levashov, P. R.

2018-01-01

In this work, structural and thermodynamic properties of a solid and liquid Ni-Al compound are studied using an ab initio method of quantum molecular dynamics (QMD). Simulations were carried out in 700-3000 K temperature range at atmospheric pressure. Radial distribution functions are analyzed to determine the presence of Ni-Al chemical bonds. Diffusion coefficients for individual components are also calculated. Another goal of this work is the investigation of the reaction propagation in thermally-initiated Ni-Al foils. For this purpose, we performed QMD simulations of Ni-Al layers in the microcanonical ensemble. An exothermic reaction between the solid Ni-Al layers is observed in our simulations at temperature less than the melting temperatures of the components.

Exploring the nonequilibrium dynamics of ultracold quantum gases by using numerical tools

NASA Astrophysics Data System (ADS)

Heidrich-Meisner, Fabian

Numerical tools such as exact diagonalization or the density matrix renormalization group method have been vital for the study of the nonequilibrium dynamics of strongly correlated many-body systems. Moreover, they provided unique insight for the interpretation of quantum gas experiments, whenever a direct comparison with theory is possible. By considering the example of the experiment by Ronzheimer et al., in which both an interaction quench and the release of bosons from a trap into an empty optical lattice (sudden expansion) was realized, I discuss several nonequilibrium effects of strongly interacting quantum gases. These include the thermalization of a closed quantum system and its connection to the eigenstate thermalization hypothesis, nonequilibrium mass transport, dynamical fermionization, and transient phenomena such as quantum distillation or dynamical quasicondensation. I highlight the role of integrability in giving rise to ballistic transport in strongly interacting 1D systems and in determining the asymptotic state after a quantum quench. The talk concludes with a perspective on open questions concerning 2D systems and the numerical simulation of their nonequilibrium dynamics. Supported by Deutsche Forschungsgemeinschaft (DFG) via FOR 801.

Quantum molecular dynamics simulation of shock-wave experiments in aluminum

NASA Astrophysics Data System (ADS)

Minakov, D. V.; Levashov, P. R.; Khishchenko, K. V.; Fortov, V. E.

2014-06-01

We present quantum molecular dynamics calculations of principal, porous, and double shock Hugoniots, release isentropes, and sound velocity behind the shock front for aluminum. A comprehensive analysis of available shock-wave data is performed; the agreement and discrepancies of simulation results with measurements are discussed. Special attention is paid to the melting region of aluminum along the principal Hugoniot; the boundaries of the melting zone are estimated using the self-diffusion coefficient. Also, we make a comparison with a high-quality multiphase equation of state for aluminum. Independent semiempirical and first-principle models are very close to each other in caloric variables (pressure, density, particle velocity, etc.) but the equation of state gives higher temperature on the principal Hugoniot and release isentropes than ab initio calculations. Thus, the quantum molecular dynamics method can be used for calibration of semiempirical equations of state in case of lack of experimental data.

Quantum molecular dynamics simulation of shock-wave experiments in aluminum

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

Minakov, D. V.; Khishchenko, K. V.; Fortov, V. E.

2014-06-14

We present quantum molecular dynamics calculations of principal, porous, and double shock Hugoniots, release isentropes, and sound velocity behind the shock front for aluminum. A comprehensive analysis of available shock-wave data is performed; the agreement and discrepancies of simulation results with measurements are discussed. Special attention is paid to the melting region of aluminum along the principal Hugoniot; the boundaries of the melting zone are estimated using the self-diffusion coefficient. Also, we make a comparison with a high-quality multiphase equation of state for aluminum. Independent semiempirical and first-principle models are very close to each other in caloric variables (pressure, density,more » particle velocity, etc.) but the equation of state gives higher temperature on the principal Hugoniot and release isentropes than ab initio calculations. Thus, the quantum molecular dynamics method can be used for calibration of semiempirical equations of state in case of lack of experimental data.« less

Quantum versus classical dynamics in the optical centrifuge

NASA Astrophysics Data System (ADS)

Armon, Tsafrir; Friedland, Lazar

2017-09-01

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

Does ℏ play a role in multidimensional spectroscopy? Reduced hierarchy equations of motion approach to molecular vibrations.

PubMed

Sakurai, Atsunori; Tanimura, Yoshitaka

2011-04-28

To investigate the role of quantum effects in vibrational spectroscopies, we have carried out numerically exact calculations of linear and nonlinear response functions for an anharmonic potential system nonlinearly coupled to a harmonic oscillator bath. Although one cannot carry out the quantum calculations of the response functions with full molecular dynamics (MD) simulations for a realistic system which consists of many molecules, it is possible to grasp the essence of the quantum effects on the vibrational spectra by employing a model Hamiltonian that describes an intra- or intermolecular vibrational motion in a condensed phase. The present model fully includes vibrational relaxation, while the stochastic model often used to simulate infrared spectra does not. We have employed the reduced quantum hierarchy equations of motion approach in the Wigner space representation to deal with nonperturbative, non-Markovian, and nonsecular system-bath interactions. Taking the classical limit of the hierarchy equations of motion, we have obtained the classical equations of motion that describe the classical dynamics under the same physical conditions as in the quantum case. By comparing the classical and quantum mechanically calculated linear and multidimensional spectra, we found that the profiles of spectra for a fast modulation case were similar, but different for a slow modulation case. In both the classical and quantum cases, we identified the resonant oscillation peak in the spectra, but the quantum peak shifted to the red compared with the classical one if the potential is anharmonic. The prominent quantum effect is the 1-2 transition peak, which appears only in the quantum mechanically calculated spectra as a result of anharmonicity in the potential or nonlinearity of the system-bath coupling. While the contribution of the 1-2 transition is negligible in the fast modulation case, it becomes important in the slow modulation case as long as the amplitude of the frequency fluctuation is small. Thus, we observed a distinct difference between the classical and quantum mechanically calculated multidimensional spectra in the slow modulation case where spectral diffusion plays a role. This fact indicates that one may not reproduce the experimentally obtained multidimensional spectrum for high-frequency vibrational modes based on classical molecular dynamics simulations if the modulation that arises from surrounding molecules is weak and slow. A practical way to overcome the difference between the classical and quantum simulations was discussed.

Towards the simulation of molecular collisions with a superconducting quantum computer

NASA Astrophysics Data System (ADS)

Geller, Michael

2013-05-01

I will discuss the prospects for the use of large-scale, error-corrected quantum computers to simulate complex quantum dynamics such as molecular collisions. This will likely require millions qubits. I will also discuss an alternative approach [M. R. Geller et al., arXiv:1210.5260] that is ideally suited for today's superconducting circuits, which uses the single-excitation subspace (SES) of a system of n tunably coupled qubits. The SES method allows many operations in the unitary group SU(n) to be implemented in a single step, bypassing the need for elementary gates, thereby making large computations possible without error correction. The method enables universal quantum simulation, including simulation of the time-dependent Schrodinger equation, and we argue that a 1000-qubit SES processor should be capable of achieving quantum speedup relative to a petaflop supercomputer. We speculate on the utility and practicality of such a simulator for atomic and molecular collision physics. Work supported by the US National Science Foundation CDI program.

Two-dimensional lattice gauge theories with superconducting quantum circuits

PubMed Central

Marcos, D.; Widmer, P.; Rico, E.; Hafezi, M.; Rabl, P.; Wiese, U.-J.; Zoller, P.

2014-01-01

A quantum simulator of U(1) lattice gauge theories can be implemented with superconducting circuits. This allows the investigation of confined and deconfined phases in quantum link models, and of valence bond solid and spin liquid phases in quantum dimer models. Fractionalized confining strings and the real-time dynamics of quantum phase transitions are accessible as well. Here we show how state-of-the-art superconducting technology allows us to simulate these phenomena in relatively small circuit lattices. By exploiting the strong non-linear couplings between quantized excitations emerging when superconducting qubits are coupled, we show how to engineer gauge invariant Hamiltonians, including ring-exchange and four-body Ising interactions. We demonstrate that, despite decoherence and disorder effects, minimal circuit instances allow us to investigate properties such as the dynamics of electric flux strings, signaling confinement in gauge invariant field theories. The experimental realization of these models in larger superconducting circuits could address open questions beyond current computational capability. PMID:25512676

Electron-phonon thermalization in a scalable method for real-time quantum dynamics

DOE PAGES

Rizzi, Valerio; Todorov, Tchavdar N.; Kohanoff, Jorge J.; ...

2016-01-27

Here, we present a quantum simulation method that follows the dynamics of out-of-equilibrium many-body systems of electrons and oscillators in real time. Its cost is linear in the number of oscillators and it can probe time scales from attoseconds to hundreds of picoseconds. Contrary to Ehrenfest dynamics, it can thermalize starting from a variety of initial conditions, including electronic population inversion. While an electronic temperature can be defined in terms of a nonequilibrium entropy, a Fermi-Dirac distribution in general emerges only after thermalization. These results can be used to construct a kinetic model of electron-phonon equilibration based on the explicitmore » quantum dynamics.« less

Dynamics of Photoexcited State of Semiconductor Quantum Dots

NASA Astrophysics Data System (ADS)

Trivedi, Dhara J.

In this thesis, non-adiabatic molecular dynamics (NAMD) of excited states in semiconductor quantum dots are investigated. Nanoscale systems provide important opportunities for theory and computation for research because the experimental tools often provide an incomplete picture of the structure and/or function of nanomaterials, and theory can often fill in missing features crucial in understanding what is being measured. The simulation of NAMD is an indispensable tool for understanding complex ultrafast photoinduced processes such as charge and energy transfer, thermal relaxation, and charge recombination. Based on the state-of-the-art ab initio approaches in both the energy and time domains, the thesis presents a comprehensive discussion of the dynamical processes in quantum dots, ranging from the initial photon absorption to the final emission. We investigate the energy relaxation and transfer rates in pure and surface passivated quantum dots of different sizes. The study establishes the fundamental mechanisms of the electron and hole relaxation processes with and without hole traps. We develop and implement more accurate and efficient methods for NAMD. These methods are advantageous over the traditional ones when one encounters classically forbidden transitions. We also explore the effect of decoherence and non-adiabatic couplings on the dynamics. The results indicate significant influence on the accuracy and related computational cost of the simulated dynamics.

Arrays of individually controlled ions suitable for two-dimensional quantum simulations

PubMed Central

Mielenz, Manuel; Kalis, Henning; Wittemer, Matthias; Hakelberg, Frederick; Warring, Ulrich; Schmied, Roman; Blain, Matthew; Maunz, Peter; Moehring, David L.; Leibfried, Dietrich; Schaetz, Tobias

2016-01-01

A precisely controlled quantum system may reveal a fundamental understanding of another, less accessible system of interest. A universal quantum computer is currently out of reach, but an analogue quantum simulator that makes relevant observables, interactions and states of a quantum model accessible could permit insight into complex dynamics. Several platforms have been suggested and proof-of-principle experiments have been conducted. Here, we operate two-dimensional arrays of three trapped ions in individually controlled harmonic wells forming equilateral triangles with side lengths 40 and 80 μm. In our approach, which is scalable to arbitrary two-dimensional lattices, we demonstrate individual control of the electronic and motional degrees of freedom, preparation of a fiducial initial state with ion motion close to the ground state, as well as a tuning of couplings between ions within experimental sequences. Our work paves the way towards a quantum simulator of two-dimensional systems designed at will. PMID:27291425

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

Shao Xiaoqiang; Wang Hongfu; Zhang Shou

We present an approach for implementation of a 1->3 orbital state quantum cloning machine based on the quantum Zeno dynamics via manipulating three rf superconducting quantum interference device (SQUID) qubits to resonantly interact with a superconducting cavity assisted by classical fields. Through appropriate modulation of the coupling constants between rf SQUIDs and classical fields, the quantum cloning machine can be realized within one step. We also discuss the effects of decoherence such as spontaneous emission and the loss of cavity in virtue of master equation. The numerical simulation result reveals that the quantum cloning machine is especially robust against themore » cavity decay, since all qubits evolve in the decoherence-free subspace with respect to cavity decay due to the quantum Zeno dynamics.« less

Modeling Quantum Dynamics in Multidimensional Systems

NASA Astrophysics Data System (ADS)

Liss, Kyle; Weinacht, Thomas; Pearson, Brett

2017-04-01

Coupling between different degrees-of-freedom is an inherent aspect of dynamics in multidimensional quantum systems. As experiments and theory begin to tackle larger molecular structures and environments, models that account for vibrational and/or electronic couplings are essential for interpretation. Relevant processes include intramolecular vibrational relaxation, conical intersections, and system-bath coupling. We describe a set of simulations designed to model coupling processes in multidimensional molecular systems, focusing on models that provide insight and allow visualization of the dynamics. Undergraduates carried out much of the work as part of a senior research project. In addition to the pedagogical value, the simulations allow for comparison between both explicit and implicit treatments of a system's many degrees-of-freedom.

Versatile microwave-driven trapped ion spin system for quantum information processing

PubMed Central

Piltz, Christian; Sriarunothai, Theeraphot; Ivanov, Svetoslav S.; Wölk, Sabine; Wunderlich, Christof

2016-01-01

Using trapped atomic ions, we demonstrate a tailored and versatile effective spin system suitable for quantum simulations and universal quantum computation. By simply applying microwave pulses, selected spins can be decoupled from the remaining system and, thus, can serve as a quantum memory, while simultaneously, other coupled spins perform conditional quantum dynamics. Also, microwave pulses can change the sign of spin-spin couplings, as well as their effective strength, even during the course of a quantum algorithm. Taking advantage of the simultaneous long-range coupling between three spins, a coherent quantum Fourier transform—an essential building block for many quantum algorithms—is efficiently realized. This approach, which is based on microwave-driven trapped ions and is complementary to laser-based methods, opens a new route to overcoming technical and physical challenges in the quest for a quantum simulator and a quantum computer. PMID:27419233

Operation of a quantum dot in the finite-state machine mode: Single-electron dynamic memory

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

Klymenko, M. V.; Klein, M.; Levine, R. D.

2016-07-14

A single electron dynamic memory is designed based on the non-equilibrium dynamics of charge states in electrostatically defined metallic quantum dots. Using the orthodox theory for computing the transfer rates and a master equation, we model the dynamical response of devices consisting of a charge sensor coupled to either a single and or a double quantum dot subjected to a pulsed gate voltage. We show that transition rates between charge states in metallic quantum dots are characterized by an asymmetry that can be controlled by the gate voltage. This effect is more pronounced when the switching between charge states correspondsmore » to a Markovian process involving electron transport through a chain of several quantum dots. By simulating the dynamics of electron transport we demonstrate that the quantum box operates as a finite-state machine that can be addressed by choosing suitable shapes and switching rates of the gate pulses. We further show that writing times in the ns range and retention memory times six orders of magnitude longer, in the ms range, can be achieved on the double quantum dot system using experimentally feasible parameters, thereby demonstrating that the device can operate as a dynamic single electron memory.« less

Can one trust quantum simulators?

PubMed

Hauke, Philipp; Cucchietti, Fernando M; Tagliacozzo, Luca; Deutsch, Ivan; Lewenstein, Maciej

2012-08-01

Various fundamental phenomena of strongly correlated quantum systems such as high-T(c) superconductivity, the fractional quantum-Hall effect and quark confinement are still awaiting a universally accepted explanation. The main obstacle is the computational complexity of solving even the most simplified theoretical models which are designed to capture the relevant quantum correlations of the many-body system of interest. In his seminal 1982 paper (Feynman 1982 Int. J. Theor. Phys. 21 467), Richard Feynman suggested that such models might be solved by 'simulation' with a new type of computer whose constituent parts are effectively governed by a desired quantum many-body dynamics. Measurements on this engineered machine, now known as a 'quantum simulator,' would reveal some unknown or difficult to compute properties of a model of interest. We argue that a useful quantum simulator must satisfy four conditions: relevance, controllability, reliability and efficiency. We review the current state of the art of digital and analog quantum simulators. Whereas so far the majority of the focus, both theoretically and experimentally, has been on controllability of relevant models, we emphasize here the need for a careful analysis of reliability and efficiency in the presence of imperfections. We discuss how disorder and noise can impact these conditions, and illustrate our concerns with novel numerical simulations of a paradigmatic example: a disordered quantum spin chain governed by the Ising model in a transverse magnetic field. We find that disorder can decrease the reliability of an analog quantum simulator of this model, although large errors in local observables are introduced only for strong levels of disorder. We conclude that the answer to the question 'Can we trust quantum simulators?' is … to some extent.

Molecular dynamics simulation of Bu4N+ in dimethylformamide: Solvation-induced volume changes

NASA Astrophysics Data System (ADS)

Kiselev, M. G.; Safonova, L. P.

2011-06-01

The structure of the Bu4N+-dimethylformamide system in the condensed and gas phases was studied by molecular dynamics simulation and quantum-chemical calculations. The calculation results were used to reveal the role played by steric effects in the volumetric characteristics of ion solvation.

Microscopic Studies of Quantum Phase Transitions in Optical Lattices

NASA Astrophysics Data System (ADS)

Bakr, Waseem S.

2011-12-01

In this thesis, I report on experiments that microscopically probe quantum phase transitions of ultracold atoms in optical lattices. We have developed a "quantum gas microscope" that allowed, for the first time, optical imaging and manipulation of single atoms in a quantum-degenerate gas on individual sites of an optical lattice. This system acts as a quantum simulator of strongly correlated materials, which are currently the subject of intense research because of the technological potential of high--T c superconductors and spintronic materials. We have used our microscope to study the superfluid to Mott insulator transition in bosons and a magnetic quantum phase transition in a spin system. In our microscopic study of the superfluid-insulator transition, we have characterized the on-site number statistics in a space- and time-resolved manner. We observed Mott insulators with fidelities as high as 99%, corresponding to entropies of 0.06kB per particle. We also measured local quantum dynamics and directly imaged the shell structure of the Mott insulator. I report on the first quantum magnetism experiments in optical lattices. We have realized a quantum Ising chain in a magnetic field, and observed a quantum phase transition between a paramagnet and antiferromagnet. We achieved strong spin interactions by encoding spins in excitations of a Mott insulator in a tilted lattice. We detected the transition by measuring the total magnetization of the system across the transition using in-situ measurements as well as the Neel ordering in the antiferromagnetic state using noise-correlation techniques. We characterized the dynamics of domain formation in the system. The spin mapping introduced opens up a new path to realizing more exotic states in optical lattices including spin liquids and quantum valence bond solids. As our system sizes become larger, simulating their physics on classical computers will require exponentially larger resources because of entanglement build-up near a quantum phase transition. We have demonstrated a quantum simulator in which all degrees of freedom can be read out microscopically, allowing the simulation of quantum many-body systems with manageable resources. More generally, the ability to image and manipulate individual atoms in optical lattices opens an avenue towards scalable quantum computation.

Statistical benchmark for BosonSampling

NASA Astrophysics Data System (ADS)

Walschaers, Mattia; Kuipers, Jack; Urbina, Juan-Diego; Mayer, Klaus; Tichy, Malte Christopher; Richter, Klaus; Buchleitner, Andreas

2016-03-01

Boson samplers—set-ups that generate complex many-particle output states through the transmission of elementary many-particle input states across a multitude of mutually coupled modes—promise the efficient quantum simulation of a classically intractable computational task, and challenge the extended Church-Turing thesis, one of the fundamental dogmas of computer science. However, as in all experimental quantum simulations of truly complex systems, one crucial problem remains: how to certify that a given experimental measurement record unambiguously results from enforcing the claimed dynamics, on bosons, fermions or distinguishable particles? Here we offer a statistical solution to the certification problem, identifying an unambiguous statistical signature of many-body quantum interference upon transmission across a multimode, random scattering device. We show that statistical analysis of only partial information on the output state allows to characterise the imparted dynamics through particle type-specific features of the emerging interference patterns. The relevant statistical quantifiers are classically computable, define a falsifiable benchmark for BosonSampling, and reveal distinctive features of many-particle quantum dynamics, which go much beyond mere bunching or anti-bunching effects.

Quantum many-body dynamics of dark solitons in optical lattices

NASA Astrophysics Data System (ADS)

Mishmash, R. V.; Danshita, I.; Clark, Charles W.; Carr, L. D.

2009-11-01

We present a fully quantum many-body treatment of dark solitons formed by ultracold bosonic atoms in one-dimensional optical lattices. Using time-evolving block decimation to simulate the single-band Bose-Hubbard Hamiltonian, we consider the quantum dynamics of density and phase engineered dark solitons as well as the quantum evolution of mean-field dark solitons injected into the quantum model. The former approach directly models how one may create quantum entangled dark solitons in experiment. While we have already presented results regarding the latter approach elsewhere [R. V. Mishmash and L. D. Carr, Phys. Rev. Lett. 103, 140403 (2009)], we expand upon those results in this work. In both cases, quantum fluctuations cause the dark soliton to fill in and may induce an inelasticity in soliton-soliton collisions. Comparisons are made to the Bogoliubov theory which predicts depletion into an anomalous mode that fills in the soliton. Our many-body treatment allows us to go beyond the Bogoliubov approximation and calculate explicitly the dynamics of the system’s natural orbitals.

Drama in Dynamics: Boom, Splash, and Speed

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

Netzloff, Heather Marie

2004-12-19

The full nature of chemistry and physics cannot be captured by static calculations alone. Dynamics calculations allow the simulation of time-dependent phenomena. This facilitates both comparisons with experimental data and the prediction and interpretation of details not easily obtainable from experiments. Simulations thus provide a direct link between theory and experiment, between microscopic details of a system and macroscopic observed properties. Many types of dynamics calculations exist. The most important distinction between the methods and the decision of which method to use can be described in terms of the size and type of molecule/reaction under consideration and the type andmore » level of accuracy required in the final properties of interest. These considerations must be balanced with available computational codes and resources as simulations to mimic ''real-life'' may require many time steps. As indicated in the title, the theme of this thesis is dynamics. The goal is to utilize the best type of dynamics for the system under study while trying to perform dynamics in the most accurate way possible. As a quantum chemist, this involves some level of first principles calculations by default. Very accurate calculations of small molecules and molecular systems are now possible with relatively high-level ab initio quantum chemistry. For example, a quantum chemical potential energy surface (PES) can be developed ''on-the-fly'' with dynamic reaction path (DRP) methods. In this way a classical trajectory is developed without prior knowledge of the PES. In order to treat solvation processes and the condensed phase, large numbers of molecules are required, especially in predicting bulk behavior. The Effective Fragment Potential (EFP) method for solvation decreases the cost of a fully quantum mechanical calculation by dividing a chemical system into an ab initio region that contains the solute and an ''effective fragment'' region that contains the remaining solvent molecules. But, despite the reduced cost relative to fully QM calculations, the EFP method, due to its complex, QM-based potential, does require more computation time than simple interaction potentials, especially when the method is used for large scale molecular dynamics simulations. Thus, the EFP method was parallelized to facilitate these calculations within the quantum chemistry program GAMESS. The EFP method provides relative energies and structures that are in excellent agreement with the analogous fully quantum results for small water clusters. The ability of the method to predict bulk water properties with a comparable accuracy is assessed by performing EFP molecular dynamics simulations. Molecular dynamics simulations can provide properties that are directly comparable with experimental results, for example radial distribution functions. The molecular PES is a fundamental starting point for chemical reaction dynamics. Many methods can be used to obtain a PES; for example, assuming a global functional form for the PES or, as mentioned above, performing ''on-the-fly'' dynamics with Al or semi-empirical calculations at every molecular configuration. But as the size of the system grows, using electronic structure theory to build a PES and, therefore, study reaction dynamics becomes virtually impossible. The program Grow builds a PES as an interpolation of Al data; the goal is to attempt to produce an accurate PES with the smallest number of Al calculations. The Grow-GAMESS interface was developed to obtain the Al data from GAMESS. Classical or quantum dynamics can be performed on the resulting surface. The interface includes the novel capability to build multi-reference PESs; these types of calculations are applicable to problems ranging from atmospheric chemistry to photochemical reaction mechanisms in organic and inorganic chemistry to fundamental biological phenomena such as photosynthesis.« less

Numerical simulations of loop quantum Bianchi-I spacetimes

NASA Astrophysics Data System (ADS)

Diener, Peter; Joe, Anton; Megevand, Miguel; Singh, Parampreet

2017-05-01

Due to the numerical complexities of studying evolution in an anisotropic quantum spacetime, in comparison to the isotropic models, the physics of loop quantized anisotropic models has remained largely unexplored. In particular, robustness of bounce and the validity of effective dynamics have so far not been established. Our analysis fills these gaps for the case of vacuum Bianchi-I spacetime. To efficiently solve the quantum Hamiltonian constraint we perform an implementation of the Cactus framework which is conventionally used for applications in numerical relativity. Using high performance computing, numerical simulations for a large number of initial states with a wide variety of fluctuations are performed. Big bang singularity is found to be replaced by anisotropic bounces for all the cases. We find that for initial states which are sharply peaked at the late times in the classical regime and bounce at a mean volume much greater than the Planck volume, effective dynamics is an excellent approximation to the underlying quantum dynamics. Departures of the effective dynamics from the quantum evolution appear for the states probing deep Planck volumes. A detailed analysis of the behavior of this departure reveals a non-monotonic and subtle dependence on fluctuations of the initial states. We find that effective dynamics in almost all of the cases underestimates the volume and hence overestimates the curvature at the bounce, a result in synergy with earlier findings in the isotropic case. The expansion and shear scalars are found to be bounded throughout the evolution.

Architectures for Quantum Simulation Showing a Quantum Speedup

NASA Astrophysics Data System (ADS)

Bermejo-Vega, Juan; Hangleiter, Dominik; Schwarz, Martin; Raussendorf, Robert; Eisert, Jens

2018-04-01

One of the main aims in the field of quantum simulation is to achieve a quantum speedup, often referred to as "quantum computational supremacy," referring to the experimental realization of a quantum device that computationally outperforms classical computers. In this work, we show that one can devise versatile and feasible schemes of two-dimensional, dynamical, quantum simulators showing such a quantum speedup, building on intermediate problems involving nonadaptive, measurement-based, quantum computation. In each of the schemes, an initial product state is prepared, potentially involving an element of randomness as in disordered models, followed by a short-time evolution under a basic translationally invariant Hamiltonian with simple nearest-neighbor interactions and a mere sampling measurement in a fixed basis. The correctness of the final-state preparation in each scheme is fully efficiently certifiable. We discuss experimental necessities and possible physical architectures, inspired by platforms of cold atoms in optical lattices and a number of others, as well as specific assumptions that enter the complexity-theoretic arguments. This work shows that benchmark settings exhibiting a quantum speedup may require little control, in contrast to universal quantum computing. Thus, our proposal puts a convincing experimental demonstration of a quantum speedup within reach in the near term.

Dirac Cellular Automaton from Split-step Quantum Walk

PubMed Central

Mallick, Arindam; Chandrashekar, C. M.

2016-01-01

Simulations of one quantum system by an other has an implication in realization of quantum machine that can imitate any quantum system and solve problems that are not accessible to classical computers. One of the approach to engineer quantum simulations is to discretize the space-time degree of freedom in quantum dynamics and define the quantum cellular automata (QCA), a local unitary update rule on a lattice. Different models of QCA are constructed using set of conditions which are not unique and are not always in implementable configuration on any other system. Dirac Cellular Automata (DCA) is one such model constructed for Dirac Hamiltonian (DH) in free quantum field theory. Here, starting from a split-step discrete-time quantum walk (QW) which is uniquely defined for experimental implementation, we recover the DCA along with all the fine oscillations in position space and bridge the missing connection between DH-DCA-QW. We will present the contribution of the parameters resulting in the fine oscillations on the Zitterbewegung frequency and entanglement. The tuneability of the evolution parameters demonstrated in experimental implementation of QW will establish it as an efficient tool to design quantum simulator and approach quantum field theory from principles of quantum information theory. PMID:27184159

A cellular automaton for the signed particle formulation of quantum mechanics

NASA Astrophysics Data System (ADS)

Sellier, J. M.; Kapanova, K. G.; Dimov, I.

2017-02-01

Recently, a new formulation of quantum mechanics, based on the concept of signed particles, has been suggested. In this paper, we introduce a cellular automaton which mimics the dynamics of quantum objects in the phase-space in a time-dependent fashion. This is twofold: it provides a simplified and accessible language to non-physicists who wants to simulate quantum mechanical systems, at the same time it enables a different way to explore the laws of Physics. Moreover, it opens the way towards hybrid simulations of quantum systems by combining full quantum models with cellular automata when the former fail. In order to show the validity of the suggested cellular automaton and its combination with the signed particle formalism, several numerical experiments are performed, showing very promising results. Being this article a preliminary study on quantum simulations in phase-space by means of cellular automata, some conclusions are drawn about the encouraging results obtained so far and the possible future developments.

Understanding quantum tunneling using diffusion Monte Carlo simulations

NASA Astrophysics Data System (ADS)

Inack, E. M.; Giudici, G.; Parolini, T.; Santoro, G.; Pilati, S.

2018-03-01

In simple ferromagnetic quantum Ising models characterized by an effective double-well energy landscape the characteristic tunneling time of path-integral Monte Carlo (PIMC) simulations has been shown to scale as the incoherent quantum-tunneling time, i.e., as 1 /Δ2 , where Δ is the tunneling gap. Since incoherent quantum tunneling is employed by quantum annealers (QAs) to solve optimization problems, this result suggests that there is no quantum advantage in using QAs with respect to quantum Monte Carlo (QMC) simulations. A counterexample is the recently introduced shamrock model (Andriyash and Amin, arXiv:1703.09277), where topological obstructions cause an exponential slowdown of the PIMC tunneling dynamics with respect to incoherent quantum tunneling, leaving open the possibility for potential quantum speedup, even for stoquastic models. In this work we investigate the tunneling time of projective QMC simulations based on the diffusion Monte Carlo (DMC) algorithm without guiding functions, showing that it scales as 1 /Δ , i.e., even more favorably than the incoherent quantum-tunneling time, both in a simple ferromagnetic system and in the more challenging shamrock model. However, a careful comparison between the DMC ground-state energies and the exact solution available for the transverse-field Ising chain indicates an exponential scaling of the computational cost required to keep a fixed relative error as the system size increases.

Removing the barrier to the calculation of activation energies

DOE PAGES

Mesele, Oluwaseun O.; Thompson, Ward H.

2016-10-06

Approaches for directly calculating the activation energy for a chemical reaction from a simulation at a single temperature are explored with applications to both classical and quantum systems. The activation energy is obtained from a time correlation function that can be evaluated from the same molecular dynamics trajectories or quantum dynamics used to evaluate the rate constant itself and thus requires essentially no extra computational work.

Out-of-time-ordered measurements as a probe of quantum dynamics

NASA Astrophysics Data System (ADS)

Bordia, Pranjal; Alet, Fabien; Hosur, Pavan

2018-03-01

Probing the out-of-equilibrium dynamics of quantum matter has gained renewed interest owing to immense experimental progress in artificial quantum systems. Dynamical quantum measures such as the growth of entanglement entropy and out-of-time-ordered correlators (OTOCs) have been shown to provide great insight by exposing subtle quantum features invisible to traditional measures such as mass transport. However, measuring them in experiments requires either identical copies of the system, an ancilla qubit coupled to the whole system, or many measurements on a single copy, thereby making scalability extremely complex and hence, severely limiting their potential. Here, we introduce an alternative quantity, the out-of-time-ordered measurement (OTOM), which involves measuring a single observable on a single copy of the system, while retaining the distinctive features of the OTOCs. We show, theoretically, that OTOMs are closely related to OTOCs in a doubled system with the same quantum statistical properties as the original system. Using exact diagonalization, we numerically simulate classical mass transport, as well as quantum dynamics through computations of the OTOC, the OTOM, and the entanglement entropy in quantum spin chain models in various interesting regimes (including chaotic and many-body localized systems). Our results demonstrate that an OTOM can successfully reveal subtle aspects of quantum dynamics hidden to classical measures and, crucially, provide experimental access to them.

Slow dynamics in translation-invariant quantum lattice models

NASA Astrophysics Data System (ADS)

Michailidis, Alexios A.; Žnidarič, Marko; Medvedyeva, Mariya; Abanin, Dmitry A.; Prosen, Tomaž; Papić, Z.

2018-03-01

Many-body quantum systems typically display fast dynamics and ballistic spreading of information. Here we address the open problem of how slow the dynamics can be after a generic breaking of integrability by local interactions. We develop a method based on degenerate perturbation theory that reveals slow dynamical regimes and delocalization processes in general translation invariant models, along with accurate estimates of their delocalization time scales. Our results shed light on the fundamental questions of the robustness of quantum integrable systems and the possibility of many-body localization without disorder. As an example, we construct a large class of one-dimensional lattice models where, despite the absence of asymptotic localization, the transient dynamics is exceptionally slow, i.e., the dynamics is indistinguishable from that of many-body localized systems for the system sizes and time scales accessible in experiments and numerical simulations.

Quantum many-body dynamics of strongly interacting atom arrays

NASA Astrophysics Data System (ADS)

Bernien, Hannes; Keesling, Alexander; Levine, Harry; Schwartz, Sylvain; Omran, Ahmed; Anschuetz, Eric; Endres, Manuel; Vuletic, Vladan; Greiner, Markus; Lukin, Mikhail

2017-04-01

The coherent interaction between large numbers of particles gives rise to fascinating quantum many-body effects and lies at the center of quantum simulations and quantum information processing. The development of systems consisting of many, well-controlled particles with tunable interactions is an outstanding challenge. Here we present a new platform based on large, reconfigurable arrays of individually trapped atoms. Strong interactions between these atoms are enabled by exciting them to Rydberg states. This flexible approach allows access to vastly different regimes with interactions tunable over several orders of magnitude. We study the coherent many-body dynamics in varying array geometries and observe the formation of Rydberg crystals.

Entanglement in Self-Supervised Dynamics

NASA Technical Reports Server (NTRS)

Zak, Michail

2011-01-01

A new type of correlation has been developed similar to quantum entanglement in self-supervised dynamics (SSD). SSDs have been introduced as a quantum-classical hybrid based upon the Madelung equation in which the quantum potential is replaced by an information potential. As a result, SSD preserves the quantum topology along with superposition, entanglement, and wave-particle duality. At the same time, it can be implemented in any scale including the Newtonian scale. The main properties of SSD associated with simulating intelligence have been formulated. The attention with this innovation is focused on intelligent agents interaction based upon the new fundamental non-New tonian effect; namely, entanglement.

Can one trust quantum simulators?

NASA Astrophysics Data System (ADS)

Hauke, Philipp; Cucchietti, Fernando M.; Tagliacozzo, Luca; Deutsch, Ivan; Lewenstein, Maciej

2012-08-01

Various fundamental phenomena of strongly correlated quantum systems such as high-Tc superconductivity, the fractional quantum-Hall effect and quark confinement are still awaiting a universally accepted explanation. The main obstacle is the computational complexity of solving even the most simplified theoretical models which are designed to capture the relevant quantum correlations of the many-body system of interest. In his seminal 1982 paper (Feynman 1982 Int. J. Theor. Phys. 21 467), Richard Feynman suggested that such models might be solved by ‘simulation’ with a new type of computer whose constituent parts are effectively governed by a desired quantum many-body dynamics. Measurements on this engineered machine, now known as a ‘quantum simulator,’ would reveal some unknown or difficult to compute properties of a model of interest. We argue that a useful quantum simulator must satisfy four conditions: relevance, controllability, reliability and efficiency. We review the current state of the art of digital and analog quantum simulators. Whereas so far the majority of the focus, both theoretically and experimentally, has been on controllability of relevant models, we emphasize here the need for a careful analysis of reliability and efficiency in the presence of imperfections. We discuss how disorder and noise can impact these conditions, and illustrate our concerns with novel numerical simulations of a paradigmatic example: a disordered quantum spin chain governed by the Ising model in a transverse magnetic field. We find that disorder can decrease the reliability of an analog quantum simulator of this model, although large errors in local observables are introduced only for strong levels of disorder. We conclude that the answer to the question ‘Can we trust quantum simulators?’ is … to some extent.

Quantum Game of Life

NASA Astrophysics Data System (ADS)

Glick, Aaron; Carr, Lincoln; Calarco, Tommaso; Montangero, Simone

2014-03-01

In order to investigate the emergence of complexity in quantum systems, we present a quantum game of life, inspired by Conway's classic game of life. Through Matrix Product State (MPS) calculations, we simulate the evolution of quantum systems, dictated by a Hamiltonian that defines the rules of our quantum game. We analyze the system through a number of measures which elicit the emergence of complexity in terms of spatial organization, system dynamics, and non-local mutual information within the network. Funded by NSF

Quantum correlation dynamics in photosynthetic processes assisted by molecular vibrations

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

Giorgi, G.L., E-mail: g.giorgi@inrim.it; Roncaglia, M.; Raffa, F.A.

2015-10-15

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

Training Schrödinger's cat: quantum optimal control. Strategic report on current status, visions and goals for research in Europe

NASA Astrophysics Data System (ADS)

Glaser, Steffen J.; Boscain, Ugo; Calarco, Tommaso; Koch, Christiane P.; Köckenberger, Walter; Kosloff, Ronnie; Kuprov, Ilya; Luy, Burkhard; Schirmer, Sophie; Schulte-Herbrüggen, Thomas; Sugny, Dominique; Wilhelm, Frank K.

2015-12-01

It is control that turns scientific knowledge into useful technology: in physics and engineering it provides a systematic way for driving a dynamical system from a given initial state into a desired target state with minimized expenditure of energy and resources. As one of the cornerstones for enabling quantum technologies, optimal quantum control keeps evolving and expanding into areas as diverse as quantum-enhanced sensing, manipulation of single spins, photons, or atoms, optical spectroscopy, photochemistry, magnetic resonance (spectroscopy as well as medical imaging), quantum information processing and quantum simulation. In this communication, state-of-the-art quantum control techniques are reviewed and put into perspective by a consortium of experts in optimal control theory and applications to spectroscopy, imaging, as well as quantum dynamics of closed and open systems. We address key challenges and sketch a roadmap for future developments.

Improving the efficiency of hierarchical equations of motion approach and application to coherent dynamics in Aharonov–Bohm interferometers

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

Hou, Dong; Xu, RuiXue; Zheng, Xiao, E-mail: xz58@ustc.edu.cn

2015-03-14

Several recent advancements for the hierarchical equations of motion (HEOM) approach are reported. First, we propose an a priori estimate for the optimal number of basis functions for the reservoir memory decomposition. Second, we make use of the sparsity of auxiliary density operators (ADOs) and propose two ansatzs to screen out all the intrinsic zero ADO elements. Third, we propose a new truncation scheme by utilizing the time derivatives of higher-tier ADOs. These novel techniques greatly reduce the memory cost of the HEOM approach, and thus enhance its efficiency and applicability. The improved HEOM approach is applied to simulate themore » coherent dynamics of Aharonov–Bohm double quantum dot interferometers. Quantitatively accurate dynamics is obtained for both noninteracting and interacting quantum dots. The crucial role of the quantum phase for the magnitude of quantum coherence and quantum entanglement is revealed.« less

Stochastic description of quantum Brownian dynamics

NASA Astrophysics Data System (ADS)

Yan, Yun-An; Shao, Jiushu

2016-08-01

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

Monte Carlo simulation of quantum Zeno effect in the brain

NASA Astrophysics Data System (ADS)

Georgiev, Danko

2015-12-01

Environmental decoherence appears to be the biggest obstacle for successful construction of quantum mind theories. Nevertheless, the quantum physicist Henry Stapp promoted the view that the mind could utilize quantum Zeno effect to influence brain dynamics and that the efficacy of such mental efforts would not be undermined by environmental decoherence of the brain. To address the physical plausibility of Stapp's claim, we modeled the brain using quantum tunneling of an electron in a multiple-well structure such as the voltage sensor in neuronal ion channels and performed Monte Carlo simulations of quantum Zeno effect exerted by the mind upon the brain in the presence or absence of environmental decoherence. The simulations unambiguously showed that the quantum Zeno effect breaks down for timescales greater than the brain decoherence time. To generalize the Monte Carlo simulation results for any n-level quantum system, we further analyzed the change of brain entropy due to the mind probing actions and proved a theorem according to which local projections cannot decrease the von Neumann entropy of the unconditional brain density matrix. The latter theorem establishes that Stapp's model is physically implausible but leaves a door open for future development of quantum mind theories provided the brain has a decoherence-free subspace.

Experimental quantum simulations of many-body physics with trapped ions.

PubMed

Schneider, Ch; Porras, Diego; Schaetz, Tobias

2012-02-01

Direct experimental access to some of the most intriguing quantum phenomena is not granted due to the lack of precise control of the relevant parameters in their naturally intricate environment. Their simulation on conventional computers is impossible, since quantum behaviour arising with superposition states or entanglement is not efficiently translatable into the classical language. However, one could gain deeper insight into complex quantum dynamics by experimentally simulating the quantum behaviour of interest in another quantum system, where the relevant parameters and interactions can be controlled and robust effects detected sufficiently well. Systems of trapped ions provide unique control of both the internal (electronic) and external (motional) degrees of freedom. The mutual Coulomb interaction between the ions allows for large interaction strengths at comparatively large mutual ion distances enabling individual control and readout. Systems of trapped ions therefore exhibit a prominent system in several physical disciplines, for example, quantum information processing or metrology. Here, we will give an overview of different trapping techniques of ions as well as implementations for coherent manipulation of their quantum states and discuss the related theoretical basics. We then report on the experimental and theoretical progress in simulating quantum many-body physics with trapped ions and present current approaches for scaling up to more ions and more-dimensional systems.

Recursive Factorization of the Inverse Overlap Matrix in Linear-Scaling Quantum Molecular Dynamics Simulations.

PubMed

Negre, Christian F A; Mniszewski, Susan M; Cawkwell, Marc J; Bock, Nicolas; Wall, Michael E; Niklasson, Anders M N

2016-07-12

We present a reduced complexity algorithm to compute the inverse overlap factors required to solve the generalized eigenvalue problem in a quantum-based molecular dynamics (MD) simulation. Our method is based on the recursive, iterative refinement of an initial guess of Z (inverse square root of the overlap matrix S). The initial guess of Z is obtained beforehand by using either an approximate divide-and-conquer technique or dynamical methods, propagated within an extended Lagrangian dynamics from previous MD time steps. With this formulation, we achieve long-term stability and energy conservation even under the incomplete, approximate, iterative refinement of Z. Linear-scaling performance is obtained using numerically thresholded sparse matrix algebra based on the ELLPACK-R sparse matrix data format, which also enables efficient shared-memory parallelization. As we show in this article using self-consistent density-functional-based tight-binding MD, our approach is faster than conventional methods based on the diagonalization of overlap matrix S for systems as small as a few hundred atoms, substantially accelerating quantum-based simulations even for molecular structures of intermediate size. For a 4158-atom water-solvated polyalanine system, we find an average speedup factor of 122 for the computation of Z in each MD step.

Recursive Factorization of the Inverse Overlap Matrix in Linear Scaling Quantum Molecular Dynamics Simulations

DOE PAGES

Negre, Christian F. A; Mniszewski, Susan M.; Cawkwell, Marc Jon; ...

2016-06-06

We present a reduced complexity algorithm to compute the inverse overlap factors required to solve the generalized eigenvalue problem in a quantum-based molecular dynamics (MD) simulation. Our method is based on the recursive iterative re nement of an initial guess Z of the inverse overlap matrix S. The initial guess of Z is obtained beforehand either by using an approximate divide and conquer technique or dynamically, propagated within an extended Lagrangian dynamics from previous MD time steps. With this formulation, we achieve long-term stability and energy conservation even under incomplete approximate iterative re nement of Z. Linear scaling performance ismore » obtained using numerically thresholded sparse matrix algebra based on the ELLPACK-R sparse matrix data format, which also enables e cient shared memory parallelization. As we show in this article using selfconsistent density functional based tight-binding MD, our approach is faster than conventional methods based on the direct diagonalization of the overlap matrix S for systems as small as a few hundred atoms, substantially accelerating quantum-based simulations even for molecular structures of intermediate size. For a 4,158 atom water-solvated polyalanine system we nd an average speedup factor of 122 for the computation of Z in each MD step.« less

Will water act as a photocatalyst for cluster phase chemical reactions? Vibrational overtone-induced dehydration reaction of methanediol

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

Kramer, Zeb C.; Takahashi, Kaito; Skodje, Rex T.

2012-04-28

The possibility of water catalysis in the vibrational overtone-induced dehydration reaction of methanediol is investigated using ab initio dynamical simulations of small methanediol-water clusters. Quantum chemistry calculations employing clusters with one or two water molecules reveal that the barrier to dehydration is lowered by over 20 kcal/mol because of hydrogen-bonding at the transition state. Nevertheless, the simulations of the reaction dynamics following OH-stretch excitation show little catalytic effect of water and, in some cases, even show an anticatalytic effect. The quantum yield for the dehydration reaction exhibits a delayed threshold effect where reaction does not occur until the photon energymore » is far above the barrier energy. Unlike thermally induced reactions, it is argued that competition between reaction and the irreversible dissipation of photon energy may be expected to raise the dynamical threshold for the reaction above the transition state energy. It is concluded that quantum chemistry calculations showing barrier lowering are not sufficient to infer water catalysis in photochemical reactions, which instead require dynamical modeling.« less

Digital-analog quantum simulation of generalized Dicke models with superconducting circuits

NASA Astrophysics Data System (ADS)

Lamata, Lucas

2017-03-01

We propose a digital-analog quantum simulation of generalized Dicke models with superconducting circuits, including Fermi- Bose condensates, biased and pulsed Dicke models, for all regimes of light-matter coupling. We encode these classes of problems in a set of superconducting qubits coupled with a bosonic mode implemented by a transmission line resonator. Via digital-analog techniques, an efficient quantum simulation can be performed in state-of-the-art circuit quantum electrodynamics platforms, by suitable decomposition into analog qubit-bosonic blocks and collective single-qubit pulses through digital steps. Moreover, just a single global analog block would be needed during the whole protocol in most of the cases, superimposed with fast periodic pulses to rotate and detune the qubits. Therefore, a large number of digital steps may be attained with this approach, providing a reduced digital error. Additionally, the number of gates per digital step does not grow with the number of qubits, rendering the simulation efficient. This strategy paves the way for the scalable digital-analog quantum simulation of many-body dynamics involving bosonic modes and spin degrees of freedom with superconducting circuits.

Digital-analog quantum simulation of generalized Dicke models with superconducting circuits

PubMed Central

Lamata, Lucas

2017-01-01

We propose a digital-analog quantum simulation of generalized Dicke models with superconducting circuits, including Fermi- Bose condensates, biased and pulsed Dicke models, for all regimes of light-matter coupling. We encode these classes of problems in a set of superconducting qubits coupled with a bosonic mode implemented by a transmission line resonator. Via digital-analog techniques, an efficient quantum simulation can be performed in state-of-the-art circuit quantum electrodynamics platforms, by suitable decomposition into analog qubit-bosonic blocks and collective single-qubit pulses through digital steps. Moreover, just a single global analog block would be needed during the whole protocol in most of the cases, superimposed with fast periodic pulses to rotate and detune the qubits. Therefore, a large number of digital steps may be attained with this approach, providing a reduced digital error. Additionally, the number of gates per digital step does not grow with the number of qubits, rendering the simulation efficient. This strategy paves the way for the scalable digital-analog quantum simulation of many-body dynamics involving bosonic modes and spin degrees of freedom with superconducting circuits. PMID:28256559

Sampling enhancement for the quantum mechanical potential based molecular dynamics simulations: a general algorithm and its extension for free energy calculation on rugged energy surface.

PubMed

Li, Hongzhi; Yang, Wei

2007-03-21

An approach is developed in the replica exchange framework to enhance conformational sampling for the quantum mechanical (QM) potential based molecular dynamics simulations. Importantly, with our enhanced sampling treatment, a decent convergence for electronic structure self-consistent-field calculation is robustly guaranteed, which is made possible in our replica exchange design by avoiding direct structure exchanges between the QM-related replicas and the activated (scaled by low scaling parameters or treated with high "effective temperatures") molecular mechanical (MM) replicas. Although the present approach represents one of the early efforts in the enhanced sampling developments specifically for quantum mechanical potentials, the QM-based simulations treated with the present technique can possess the similar sampling efficiency to the MM based simulations treated with the Hamiltonian replica exchange method (HREM). In the present paper, by combining this sampling method with one of our recent developments (the dual-topology alchemical HREM approach), we also introduce a method for the sampling enhanced QM-based free energy calculations.

Quantum Engineering of Dynamical Gauge Fields on Optical Lattices

DTIC Science & Technology

2016-07-08

opens the door for exciting new research directions, such as quantum simulation of the Schwinger model and of non-Abelian models. (a) Papers...exact blocking formulas from the TRG formulation of the transfer matrix. The second is a worm algorithm. The particle number distributions obtained...a fact that can be explained by an approximate particle- hole symmetry. We have also developed a computer code suite for simulating the Abelian

Nuclear quantum dynamics in dense hydrogen

PubMed Central

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

2014-01-01

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

Dynamic electron-ion collisions and nuclear quantum effects in quantum simulation of warm dense matter.

PubMed

Kang, Dongdong; Dai, Jiayu

2018-02-21

The structural, thermodynamic and transport properties of warm dense matter (WDM) are crucial to the fields of astrophysics and planet science, as well as inertial confinement fusion. WDM refers to the states of matter in a regime of temperature and density between cold condensed matter and hot ideal plasmas, where the density is from near-solid up to ten times solid density, and the temperature between 0.1 and 100 eV. In the WDM regime, matter exhibits moderately or strongly coupled, partially degenerate properties. Therefore, the methods used to deal with condensed matter and isolated atoms need to be properly validated for WDM. It is therefore a big challenge to understand WDM within a unified theoretical description with reliable accuracy. Here, we review the progress in the theoretical study of WDM with state-of-the-art simulations, i.e. quantum Langevin molecular dynamics and first principles path integral molecular dynamics. The related applications for WDM are also included.

Dynamic electron-ion collisions and nuclear quantum effects in quantum simulation of warm dense matter

NASA Astrophysics Data System (ADS)

Kang, Dongdong; Dai, Jiayu

2018-02-01

The structural, thermodynamic and transport properties of warm dense matter (WDM) are crucial to the fields of astrophysics and planet science, as well as inertial confinement fusion. WDM refers to the states of matter in a regime of temperature and density between cold condensed matter and hot ideal plasmas, where the density is from near-solid up to ten times solid density, and the temperature between 0.1 and 100 eV. In the WDM regime, matter exhibits moderately or strongly coupled, partially degenerate properties. Therefore, the methods used to deal with condensed matter and isolated atoms need to be properly validated for WDM. It is therefore a big challenge to understand WDM within a unified theoretical description with reliable accuracy. Here, we review the progress in the theoretical study of WDM with state-of-the-art simulations, i.e. quantum Langevin molecular dynamics and first principles path integral molecular dynamics. The related applications for WDM are also included.

The quantum CP-violating kaon system reproduced in the electronic laboratory

NASA Astrophysics Data System (ADS)

Caruso, M.; Fanchiotti, H.; García Canal, C. A.; Mayosky, M.; Veiga, A.

2016-11-01

The equivalence between the Schrödinger dynamics of a quantum system with a finite number of basis states and a classical dynamics is realized in terms of electric networks. The isomorphism that connects in a univocal way both dynamical systems was applied to the case of neutral mesons, kaons in particular, and the class of electric networks univocally related to the quantum system was analysed. Moreover, under CPT invariance, the relevant ɛ parameter that measures CP violation in the kaon system is reinterpreted in terms of network parameters. All these results were explicitly shown by means of both a numerical simulation of the implied networks and by constructing the corresponding circuits.

Arrays of individually controlled ions suitable for two-dimensional quantum simulations

DOE PAGES

Mielenz, Manuel; Kalis, Henning; Wittemer, Matthias; ...

2016-06-13

A precisely controlled quantum system may reveal a fundamental understanding of another, less accessible system of interest. A universal quantum computer is currently out of reach, but an analogue quantum simulator that makes relevant observables, interactions and states of a quantum model accessible could permit insight into complex dynamics. Several platforms have been suggested and proof-of-principle experiments have been conducted. Here, we operate two-dimensional arrays of three trapped ions in individually controlled harmonic wells forming equilateral triangles with side lengths 40 and 80 μm. In our approach, which is scalable to arbitrary two-dimensional lattices, we demonstrate individual control of themore » electronic and motional degrees of freedom, preparation of a fiducial initial state with ion motion close to the ground state, as well as a tuning of couplings between ions within experimental sequences. Lastly, our work paves the way towards a quantum simulator of two-dimensional systems designed at will.« less

Experimentally simulating the dynamics of quantum light and matter at ultrastrong coupling using circuit QED (2) - light dynamics and light-matter entanglement -

NASA Astrophysics Data System (ADS)

Sagastizabal, R.; Langford, N. K.; Kounalakis, M.; Dickel, C.; Bruno, A.; Luthi, F.; Thoen, D. J.; Endo, A.; Dicarlo, L.

Light-matter interaction can lead to large photon build-up and hybrid atom-photon entanglement in the ultrastrong coupling (USC) regime, where the coupling strength becomes comparable to the eigenenergies of the system. Accessing the cavity degree of freedom, however, is an outstanding challenge in natural USC systems. In this talk, we directly probe light field dynamics in the USC regime using a digital simulation of the quantum Rabi model in a planar circuit QED chip with a transmon moderately coupled to a resonator. We produce high-accuracy USC light-matter dynamics, using second-order Trotterisation and up to 90 Trotter steps. We probe the average photon number, photon parity and perform Wigner tomography of the simulated field. Finally, we combine tomography of the resonator with qubit measurements to evidence the Schrödinger-cat-like atom-photon entanglement which is a key signature of light-matter dynamics in the USC regime. Funding from the EU FP7 Project ScaleQIT, the ERC Synergy Grant QC-lab, the Netherlands Organization of Scientic Research (NWO), and Microsoft Research.

QuantumOptics.jl: A Julia framework for simulating open quantum systems

NASA Astrophysics Data System (ADS)

Krämer, Sebastian; Plankensteiner, David; Ostermann, Laurin; Ritsch, Helmut

2018-06-01

We present an open source computational framework geared towards the efficient numerical investigation of open quantum systems written in the Julia programming language. Built exclusively in Julia and based on standard quantum optics notation, the toolbox offers speed comparable to low-level statically typed languages, without compromising on the accessibility and code readability found in dynamic languages. After introducing the framework, we highlight its features and showcase implementations of generic quantum models. Finally, we compare its usability and performance to two well-established and widely used numerical quantum libraries.

Tensor network methods for the simulation of open quantum dynamics in multichromophore systems: Application to singlet fission in novel pentacene dimers

NASA Astrophysics Data System (ADS)

Chin, Alex

Singlet fission (SF) is an ultrafast process in which a singlet exciton spontaneously converts into a pair of entangled triplet excitons on neighbouring organic molecules. As a mechanism of multiple exciton generation, it has been suggested as a way to increase the efficiency of organic photovoltaic devices, and its underlying photophysics across a wide range of molecules and materials has attracted significant theoretical attention. Recently, a number of studies using ultrafast nonlinear optics have underscored the importance of intramolecular vibrational dynamics in efficient SF systems, prompting a need for methods capable of simulating open quantum dynamics in the presence of highly structured and strongly coupled environments. Here, a combination of ab initio electronic structure techniques and a new tensor-network methodology for simulating open vibronic dynamics is presented and applied to a recently synthesised dimer of pentacene (DP-Mes). We show that ultrafast (300 fs) SF in this system is driven entirely by symmetry breaking vibrations, and our many-body approach enables the real-time identification and tracking of the ''functional' vibrational dynamics and the role of the ''bath''-like parts of the environment. Deeper analysis of the emerging wave functions points to interesting links between the time at which parts of the environment become relevant to the SF process and the optimal topology of the tensor networks, highlighting the additional insight provided by moving the problem into the natural language of correlated quantum states and how this could lead to simulations of much larger multichromophore systems Supported by The Winton Programme for the Physics of Sustainability.

Surface Modification Engineered Assembly of Novel Quantum Dot Architectures for Advanced Applications

DTIC Science & Technology

2008-02-09

Campbell, S. Ogata, and F. Shimojo, “ Multimillion atom simulations of nanosystems on parallel computers,” in Proceedings of the International...nanomesas: multimillion -atom molecular dynamics simulations on parallel computers,” J. Appl. Phys. 94, 6762 (2003). 21. P. Vashishta, R. K. Kalia...and A. Nakano, “ Multimillion atom molecular dynamics simulations of nanoparticles on parallel computers,” Journal of Nanoparticle Research 5, 119-135

Mechanistic Insights into Radical-Mediated Oxidation of Tryptophan from ab Initio Quantum Chemistry Calculations and QM/MM Molecular Dynamics Simulations.

PubMed

Wood, Geoffrey P F; Sreedhara, Alavattam; Moore, Jamie M; Wang, John; Trout, Bernhardt L

2016-05-12

An assessment of the mechanisms of (•)OH and (•)OOH radical-mediated oxidation of tryptophan was performed using density functional theory calculations and ab initio plane-wave Quantum Mechanics/Molecular Mechanics (QM/MM) molecular dynamics simulations. For the (•)OH reactions, addition to the pyrrole ring at position 2 is the most favored site with a barrierless reaction in the gas phase. The subsequent degradation of this adduct through a H atom transfer to water was intermittently observed in aqueous-phase molecular dynamics simulations. For the (•)OOH reactions, addition to the pyrrole ring at position 2 is the most favored pathway, in contrast to the situation in the model system ethylene, where concerted addition to the double bond is preferred. From the (•)OOH position 2 adduct QM/MM simulations show that formation of oxy-3-indolanaline occurs readily in an aqueous environment. The observed transformation starts from an initial rupture of the O-O bond followed by a H atom transfer with the accompanying loss of an (•)OH radical to solution. Finally, classical molecular dynamics simulations were performed to equate observed differential oxidation rates of various tryptophan residues in monoclonal antibody fragments. It was found that simple parameters derived from simulation correlate well with the experimental data.

Quantum-like dynamics of decision-making

NASA Astrophysics Data System (ADS)

Asano, Masanari; Basieva, Irina; Khrennikov, Andrei; Ohya, Masanori; Tanaka, Yoshiharu

2012-03-01

In cognitive psychology, some experiments for games were reported, and they demonstrated that real players did not use the “rational strategy” provided by classical game theory and based on the notion of the Nasch equilibrium. This psychological phenomenon was called the disjunction effect. Recently, we proposed a model of decision making which can explain this effect (“irrationality” of players) Asano et al. (2010, 2011) [23,24]. Our model is based on the mathematical formalism of quantum mechanics, because psychological fluctuations inducing the irrationality are formally represented as quantum fluctuations Asano et al. (2011) [55]. In this paper, we reconsider the process of quantum-like decision-making more closely and redefine it as a well-defined quantum dynamics by using the concept of lifting channel, which is an important concept in quantum information theory. We also present numerical simulation for this quantum-like mental dynamics. It is non-Markovian by its nature. Stabilization to the steady state solution (determining subjective probabilities for decision making) is based on the collective effect of mental fluctuations collected in the working memory of a decision maker.

Shortcuts to adiabatic passage for fast generation of Greenberger-Horne-Zeilinger states by transitionless quantum driving.

PubMed

Chen, Ye-Hong; Xia, Yan; Song, Jie; Chen, Qing-Qin

2015-10-28

Berry's approach on "transitionless quantum driving" shows how to set a Hamiltonian which drives the dynamics of a system along instantaneous eigenstates of a reference Hamiltonian to reproduce the same final result of an adiabatic process in a shorter time. In this paper, motivated by transitionless quantum driving, we construct shortcuts to adiabatic passage in a three-atom system to create the Greenberger-Horne-Zeilinger states with the help of quantum Zeno dynamics and of non-resonant lasers. The influence of various decoherence processes is discussed by numerical simulation and the result proves that the scheme is fast and robust against decoherence and operational imperfection.

Quasi-classical approaches to vibronic spectra revisited

NASA Astrophysics Data System (ADS)

Karsten, Sven; Ivanov, Sergei D.; Bokarev, Sergey I.; Kühn, Oliver

2018-03-01

The framework to approach quasi-classical dynamics in the electronic ground state is well established and is based on the Kubo-transformed time correlation function (TCF), being the most classical-like quantum TCF. Here we discuss whether the choice of the Kubo-transformed TCF as a starting point for simulating vibronic spectra is as unambiguous as it is for vibrational ones. Employing imaginary-time path integral techniques in combination with the interaction representation allowed us to formulate a method for simulating vibronic spectra in the adiabatic regime that takes nuclear quantum effects and dynamics on multiple potential energy surfaces into account. Further, a generalized quantum TCF is proposed that contains many well-established TCFs, including the Kubo one, as particular cases. Importantly, it also provides a framework to construct new quantum TCFs. Applying the developed methodology to the generalized TCF leads to a plethora of simulation protocols, which are based on the well-known TCFs as well as on new ones. Their performance is investigated on 1D anharmonic model systems at finite temperatures. It is shown that the protocols based on the new TCFs may lead to superior results with respect to those based on the common ones. The strategies to find the optimal approach are discussed.

Molecular Dynamics Simulation of the Thermophysical Properties of Quantum Liquid Helium Using the Feynman-Hibbs Potential

NASA Astrophysics Data System (ADS)

Liu, J.; Lu, W. Q.

2010-03-01

This paper presents the detailed MD simulation on the properties including the thermal conductivities and viscosities of the quantum fluid helium at different state points. The molecular interactions are represented by the Lennard-Jones pair potentials supplemented by quantum corrections following the Feynman-Hibbs approach and the properties are calculated using the Green-Kubo equations. A comparison is made among the numerical results using LJ and QFH potentials and the existing database and shows that the LJ model is not quantitatively correct for the supercritical liquid helium, thereby the quantum effect must be taken into account when the quantum fluid helium is studied. The comparison of the thermal conductivity is also made as a function of temperatures and pressure and the results show quantum effect correction is an efficient tool to get the thermal conductivities.

Tunable two-dimensional arrays of single Rydberg atoms for realizing quantum Ising models

NASA Astrophysics Data System (ADS)

Labuhn, Henning; Barredo, Daniel; Ravets, Sylvain; de Léséleuc, Sylvain; Macrì, Tommaso; Lahaye, Thierry; Browaeys, Antoine

2016-06-01

Spin models are the prime example of simplified many-body Hamiltonians used to model complex, strongly correlated real-world materials. However, despite the simplified character of such models, their dynamics often cannot be simulated exactly on classical computers when the number of particles exceeds a few tens. For this reason, quantum simulation of spin Hamiltonians using the tools of atomic and molecular physics has become a very active field over the past years, using ultracold atoms or molecules in optical lattices, or trapped ions. All of these approaches have their own strengths and limitations. Here we report an alternative platform for the study of spin systems, using individual atoms trapped in tunable two-dimensional arrays of optical microtraps with arbitrary geometries, where filling fractions range from 60 to 100 per cent. When excited to high-energy Rydberg D states, the atoms undergo strong interactions whose anisotropic character opens the way to simulating exotic matter. We illustrate the versatility of our system by studying the dynamics of a quantum Ising-like spin-1/2 system in a transverse field with up to 30 spins, for a variety of geometries in one and two dimensions, and for a wide range of interaction strengths. For geometries where the anisotropy is expected to have small effects on the dynamics, we find excellent agreement with ab initio simulations of the spin-1/2 system, while for strongly anisotropic situations the multilevel structure of the D states has a measurable influence. Our findings establish arrays of single Rydberg atoms as a versatile platform for the study of quantum magnetism.

Nonlinear absorption dynamics using field-induced surface hopping: zinc porphyrin in water.

PubMed

Röhr, Merle I S; Petersen, Jens; Wohlgemuth, Matthias; Bonačić-Koutecký, Vlasta; Mitrić, Roland

2013-05-10

We wish to present the application of our field-induced surface-hopping (FISH) method to simulate nonlinear absorption dynamics induced by strong nonresonant laser fields. We provide a systematic comparison of the FISH approach with exact quantum dynamics simulations on a multistate model system and demonstrate that FISH allows for accurate simulations of nonlinear excitation processes including multiphoton electronic transitions. In particular, two different approaches for simulating two-photon transitions are compared. The first approach is essentially exact and involves the solution of the time-dependent Schrödinger equation in an extended manifold of excited states, while in the second one only transiently populated nonessential states are replaced by an effective quadratic coupling term, and dynamics is performed in a considerably smaller manifold of states. We illustrate the applicability of our method to complex molecular systems by simulating the linear and nonlinear laser-driven dynamics in zinc (Zn) porphyrin in the gas phase and in water. For this purpose, the FISH approach is connected with the quantum mechanical-molecular mechanical approach (QM/MM) which is generally applicable to large classes of complex systems. Our findings that multiphoton absorption and dynamics increase the population of higher excited states of Zn porphyrin in the nonlinear regime, in particular in solution, provides a means for manipulating excited-state properties, such as transient absorption dynamics and electronic relaxation. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Chemical and quantum simulation of electron transfer through a polypeptide

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

Ungar, L.W.; Voth, G.A.; Newton, M.D.

1999-08-26

Quantum rate theory, molecular dynamics simulations, and semiempirical electronic structure calculations are used to fully investigate electron transfer mediated by a solvated polypeptide for the first time. Using a stationary-phase approximation, the nonadiabatic electron-transfer rate constant is calculated from the nuclear free energies and the electronic coupling between the initial and final states. The former are obtained from quantum path integral and classical molecular dynamics simulations; the latter are calculated using semiempirical electronic structure calculations and the generalized Mulliken-Hush method. Importantly, no parameters are fit to kinetic data. The simulated system consists of a solvated four-proline polypeptide with a tris(bipyridine)rutheniummore » donor group and an oxypentamminecobalt acceptor group. From the simulation data entropy and energy contributions to the free energies are distinguished. Quantum suppression of the barrier, including important solvent contributions, is demonstrated. Although free energy profiles along the reaction coordinate are nearly parabolic, pronounced departures from harmonic behavior are found for the separate energy and entropy functions. Harmonic models of the system are compared to simulation results in order to quantify anharmonic effects. Electronic structure calculations show that electronic coupling elements vary considerably with system conformation, even when the effective donor-acceptor separation remains roughly constant. The calculations indicate that electron transfer in a significant range of conformations linking the polypeptide to the acceptor may contribute to the overall rate constant. After correction for limitations of the solvent model, the simulations and calculations agree well with the experimental activation energy and Arrhenius prefactor.« less

The Development of Rigorously Correct, Dynamical Pseudopotentials for Use in Mixed Quantum/Classical Molecular Dynamics Simulations in the Condensed Phase

NASA Astrophysics Data System (ADS)

Kahros, Argyris

Incorporating quantum mechanics into an atomistic simulation necessarily involves solving the Schrodinger equation. Unfortunately, the computational expense associated with solving this equation scales miserably with the number of included quantum degrees of freedom (DOF). The situation is so dire, in fact, that a molecular dynamics (MD) simulation cannot include more than a small number of quantum DOFs before it becomes computationally intractable. Thus, if one were to simulate a relatively large system, such as one containing several hundred atoms or molecules, it would be unreasonable to attempt to include the effects of all of the electrons associated with all of the components of the system. The mixed quantum/classical (MQC) approach provides a way to circumvent this issue. It involves treating the vast majority of the system classically, which incurs minimal computational expense, and reserves the consideration of quantum mechanical effects for only the few degrees of freedom more directly involved in the chemical phenomenon being studied. For example, if one were to study the bonding of a single diatomic molecule in the gas phase, one could employ a MQC approach by treating the nuclei of the molecule's two atoms classically---including the deeply bound, low-energy electrons that change relatively little---and solving the Schrodinger equation only for the high energy electron(s) directly involved in the bonding of the classical cores. In such a way, one could study the bonding of this molecule in a rigorous fashion while treating only the directly related degrees of freedom quantum mechanically. Pseudopotentials are then responsible for dictating the interactions between the quantum and classical degrees of freedom. As these potentials are the sole link between the quantum and classical DOFs, their proper development is of the utmost importance. This Thesis is concerned primarily with my work on the development of novel, rigorous and dynamical pseudopotentials for use in mixed quantum/ classical simulations in the condensed phase. The pseudopotentials discussed within are constructed in an ab initio fashion, without the introduction of any empiricism, and are able to exactly reproduce the results of higher level, fully quantum mechanical Hartree-Fock calculations. A recurring theme in the following pages is overcoming the so-called frozen core approximation (FCA). This essentially comes down to creating pseudopotentials that are able to respond in some way to the local molecular environment in a rigorous fashion. The various methods and discussions that are part of this document are presented in the context of two particular systems. The first is the sodium dimer cation molecule, which serves as a proof of concept for the development of coordinate-dependent pseudopotentials and is the subject of Chapters 2 and 3. Next, the hydrated electron---the excess electron in liquid water---is tackled in an effort to address the recent controversy concerning its true structure and is the subject of Chapters 4 and 5. In essence, the work in this Dissertation is concerned with finding new ways to overcome the problem of a lack of infinite computer processing power.

Molecular Dynamics Simulations of Nucleic Acids. From Tetranucleotides to the Ribosome.

PubMed

Šponer, Jiří; Banáš, Pavel; Jurečka, Petr; Zgarbová, Marie; Kührová, Petra; Havrila, Marek; Krepl, Miroslav; Stadlbauer, Petr; Otyepka, Michal

2014-05-15

We present a brief overview of explicit solvent molecular dynamics (MD) simulations of nucleic acids. We explain physical chemistry limitations of the simulations, namely, the molecular mechanics (MM) force field (FF) approximation and limited time scale. Further, we discuss relations and differences between simulations and experiments, compare standard and enhanced sampling simulations, discuss the role of starting structures, comment on different versions of nucleic acid FFs, and relate MM computations with contemporary quantum chemistry. Despite its limitations, we show that MD is a powerful technique for studying the structural dynamics of nucleic acids with a fast growing potential that substantially complements experimental results and aids their interpretation.

Competing quantum effects in the free energy profiles and diffusion rates of hydrogen and deuterium molecules through clathrate hydrates.

PubMed

Cendagorta, Joseph R; Powers, Anna; Hele, Timothy J H; Marsalek, Ondrej; Bačić, Zlatko; Tuckerman, Mark E

2016-11-30

Clathrate hydrates hold considerable promise as safe and economical materials for hydrogen storage. Here we present a quantum mechanical study of H 2 and D 2 diffusion through a hexagonal face shared by two large cages of clathrate hydrates over a wide range of temperatures. Path integral molecular dynamics simulations are used to compute the free-energy profiles for the diffusion of H 2 and D 2 as a function of temperature. Ring polymer molecular dynamics rate theory, incorporating both exact quantum statistics and approximate quantum dynamical effects, is utilized in the calculations of the H 2 and D 2 diffusion rates in a broad temperature interval. We find that the shape of the quantum free-energy profiles and their height relative to the classical free energy barriers at a given temperature, as well as the rate of diffusion, are strongly affected by competing quantum effects: above 25 K, zero-point energy (ZPE) perpendicular to the reaction path for diffusion between cavities decreases the quantum rate compared to the classical rate, whereas at lower temperatures tunneling outcompetes the ZPE and as a result the quantum rate is greater than the classical rate.

| NREL

Science.gov Websites

of NREL's Computational Science Center, where he uses electronic structure calculations and other introductory chemistry and physical chemistry. Research Interests Electronic structure and dynamics in the quantum/classical molecular dynamics simulation|Coupling of molecular electronic structure to

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.

Ab initio implementation of quantum trajectory mean-field approach and dynamical simulation of the N{sub 2}CO photodissociation

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

Xie, Binbin; Liu, Lihong; Cui, Ganglong

2015-11-21

In this work, the recently introduced quantum trajectory mean-field (QTMF) approach is implemented and employed to explore photodissociation dynamics of diazirinone (N{sub 2}CO), which are based on the high-level ab initio calculation. For comparison, the photodissociation process has been simulated as well with the fewest-switches surface hopping (FSSH) and the ab initio multiple spawning (AIMS) methods. Overall, the dynamical behavior predicted by the three methods is consistent. The N{sub 2}CO photodissociation at λ > 335 nm is an ultrafast process and the two C—N bonds are broken in a stepwise way, giving birth to CO and N{sub 2} as themore » final products in the ground state. Meanwhile, some noticeable differences were found in the QTMF, FSSH, and AIMS simulated time constants for fission of the C—N bonds, excited-state lifetime, and nonadiabatic transition ratios in different intersection regions. These have been discussed in detail. The present study provides a clear evidence that direct ab initio QTMF approach is one of the reliable tools for simulating nonadiabatic dynamics processes.« less

Polynomial-time quantum algorithm for the simulation of chemical dynamics

PubMed Central

Kassal, Ivan; Jordan, Stephen P.; Love, Peter J.; Mohseni, Masoud; Aspuru-Guzik, Alán

2008-01-01

The computational cost of exact methods for quantum simulation using classical computers grows exponentially with system size. As a consequence, these techniques can be applied only to small systems. By contrast, we demonstrate that quantum computers could exactly simulate chemical reactions in polynomial time. Our algorithm uses the split-operator approach and explicitly simulates all electron-nuclear and interelectronic interactions in quadratic time. Surprisingly, this treatment is not only more accurate than the Born–Oppenheimer approximation but faster and more efficient as well, for all reactions with more than about four atoms. This is the case even though the entire electronic wave function is propagated on a grid with appropriately short time steps. Although the preparation and measurement of arbitrary states on a quantum computer is inefficient, here we demonstrate how to prepare states of chemical interest efficiently. We also show how to efficiently obtain chemically relevant observables, such as state-to-state transition probabilities and thermal reaction rates. Quantum computers using these techniques could outperform current classical computers with 100 qubits. PMID:19033207

Probability Simulations by Non-Lipschitz Chaos

NASA Technical Reports Server (NTRS)

Zak, Michail

1996-01-01

It has been demonstrated that classical probabilities, and in particular, probabilistic Turing machine, can be simulated by combining chaos and non-Lipschitz dynamics, without utilization of any man-made devices. Self-organizing properties of systems coupling simulated and calculated probabilities and their link to quantum computations are discussed.

Quantum nuclear effects in water using centroid molecular dynamics

NASA Astrophysics Data System (ADS)

Kondratyuk, N. D.; Norman, G. E.; Stegailov, V. V.

2018-01-01

The quantum nuclear effects are studied in water using the method of centroid molecular dynamics (CMD). The aim is the calibration of CMD implementation in LAMMPS. The calculated intramolecular energy, atoms gyration radii and radial distribution functions are shown in comparison with previous works. The work is assumed to be the step toward to solution of the discrepancy between the simulation results and the experimental data of liquid n-alkane properties in our previous works.

Fluctuation Theorem for Many-Body Pure Quantum States.

PubMed

Iyoda, Eiki; Kaneko, Kazuya; Sagawa, Takahiro

2017-09-08

We prove the second law of thermodynamics and the nonequilibrium fluctuation theorem for pure quantum states. The entire system obeys reversible unitary dynamics, where the initial state of the heat bath is not the canonical distribution but is a single energy eigenstate that satisfies the eigenstate-thermalization hypothesis. Our result is mathematically rigorous and based on the Lieb-Robinson bound, which gives the upper bound of the velocity of information propagation in many-body quantum systems. The entanglement entropy of a subsystem is shown connected to thermodynamic heat, highlighting the foundation of the information-thermodynamics link. We confirmed our theory by numerical simulation of hard-core bosons, and observed dynamical crossover from thermal fluctuations to bare quantum fluctuations. Our result reveals a universal scenario that the second law emerges from quantum mechanics, and can be experimentally tested by artificial isolated quantum systems such as ultracold atoms.

Fluctuation Theorem for Many-Body Pure Quantum States

NASA Astrophysics Data System (ADS)

Iyoda, Eiki; Kaneko, Kazuya; Sagawa, Takahiro

2017-09-01

We prove the second law of thermodynamics and the nonequilibrium fluctuation theorem for pure quantum states. The entire system obeys reversible unitary dynamics, where the initial state of the heat bath is not the canonical distribution but is a single energy eigenstate that satisfies the eigenstate-thermalization hypothesis. Our result is mathematically rigorous and based on the Lieb-Robinson bound, which gives the upper bound of the velocity of information propagation in many-body quantum systems. The entanglement entropy of a subsystem is shown connected to thermodynamic heat, highlighting the foundation of the information-thermodynamics link. We confirmed our theory by numerical simulation of hard-core bosons, and observed dynamical crossover from thermal fluctuations to bare quantum fluctuations. Our result reveals a universal scenario that the second law emerges from quantum mechanics, and can be experimentally tested by artificial isolated quantum systems such as ultracold atoms.

Nuclear quantum effects in water exchange around lithium and fluoride ions

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

Wilkins, David M.; Manolopoulos, David E.; Dang, Liem X.

2015-02-14

We employ classical and ring polymer molecular dynamics simulations to study the effect of nuclear quantum fluctuations on the structure and the water exchange dynamics of aqueous solutions of lithium and fluoride ions. While we obtain reasonably good agreement with experimental data for solutions of lithium by augmenting the Coulombic interactions between the ion and the water molecules with a standard Lennard-Jones ion-oxygen potential, the same is not true for solutions of fluoride, for which we find that a potential with a softer repulsive wall gives much better agreement. A small degree of destabilization of the first hydration shell ismore » found in quantum simulations of both ions when compared with classical simulations, with the shell becoming less sharply defined and the mean residence time of the water molecules in the shell decreasing. In line with these modest differences, we find that the mechanisms of the exchange processes are unaffected by quantization, so a classical description of these reactions gives qualitatively correct and quantitatively reasonable results. We also find that the quantum effects in solutions of lithium are larger than in solutions of fluoride. This is partly due to the stronger interaction of lithium with water molecules, partly due to the lighter mass of lithium and partly due to competing quantum effects in the hydration of fluoride, which are absent in the hydration of lithium.« less

Theory of atomistic simulation of spin-transfer torque in nanomagnets

NASA Astrophysics Data System (ADS)

Tay, Tiamhock; Sham, L. J.

2013-05-01

In spin-transfer torque (STT) for technological applications, the miniaturization of the magnet may reach the stage of requiring a fully quantum-mechanical treatment. We present an STT theory which uses the quantum macrospin ground and excited (magnon) states of the nanomagnet. This allows for energy and angular momentum exchanges between the current electron and the nano-magnet. We develop a method of magnetization dynamics simulation which captures the heating effect on the magnet by the spin-polarized current and the temperature dependence in STT. We also discuss the magnetostatics effect on magnon scattering for ferromagnetic relaxation in a thin film. Our work demonstrates a realistic step towards simulation of quantum spin-transfer torque physics in nanoscale magnets.

Statistical moments of quantum-walk dynamics reveal topological quantum transitions.

PubMed

Cardano, Filippo; Maffei, Maria; Massa, Francesco; Piccirillo, Bruno; de Lisio, Corrado; De Filippis, Giulio; Cataudella, Vittorio; Santamato, Enrico; Marrucci, Lorenzo

2016-04-22

Many phenomena in solid-state physics can be understood in terms of their topological properties. Recently, controlled protocols of quantum walk (QW) are proving to be effective simulators of such phenomena. Here we report the realization of a photonic QW showing both the trivial and the non-trivial topologies associated with chiral symmetry in one-dimensional (1D) periodic systems. We find that the probability distribution moments of the walker position after many steps can be used as direct indicators of the topological quantum transition: while varying a control parameter that defines the system phase, these moments exhibit a slope discontinuity at the transition point. Numerical simulations strongly support the conjecture that these features are general of 1D topological systems. Extending this approach to higher dimensions, different topological classes, and other typologies of quantum phases may offer general instruments for investigating and experimentally detecting quantum transitions in such complex systems.

Statistical moments of quantum-walk dynamics reveal topological quantum transitions

PubMed Central

Cardano, Filippo; Maffei, Maria; Massa, Francesco; Piccirillo, Bruno; de Lisio, Corrado; De Filippis, Giulio; Cataudella, Vittorio; Santamato, Enrico; Marrucci, Lorenzo

2016-01-01

Many phenomena in solid-state physics can be understood in terms of their topological properties. Recently, controlled protocols of quantum walk (QW) are proving to be effective simulators of such phenomena. Here we report the realization of a photonic QW showing both the trivial and the non-trivial topologies associated with chiral symmetry in one-dimensional (1D) periodic systems. We find that the probability distribution moments of the walker position after many steps can be used as direct indicators of the topological quantum transition: while varying a control parameter that defines the system phase, these moments exhibit a slope discontinuity at the transition point. Numerical simulations strongly support the conjecture that these features are general of 1D topological systems. Extending this approach to higher dimensions, different topological classes, and other typologies of quantum phases may offer general instruments for investigating and experimentally detecting quantum transitions in such complex systems. PMID:27102945

An adaptive quantum mechanics/molecular mechanics method for the infrared spectrum of water: incorporation of the quantum effect between solute and solvent.

PubMed

Watanabe, Hiroshi C; Banno, Misa; Sakurai, Minoru

2016-03-14

Quantum effects in solute-solvent interactions, such as the many-body effect and the dipole-induced dipole, are known to be critical factors influencing the infrared spectra of species in the liquid phase. For accurate spectrum evaluation, the surrounding solvent molecules, in addition to the solute of interest, should be treated using a quantum mechanical method. However, conventional quantum mechanics/molecular mechanics (QM/MM) methods cannot handle free QM solvent molecules during molecular dynamics (MD) simulation because of the diffusion problem. To deal with this problem, we have previously proposed an adaptive QM/MM "size-consistent multipartitioning (SCMP) method". In the present study, as the first application of the SCMP method, we demonstrate the reproduction of the infrared spectrum of liquid-phase water, and evaluate the quantum effect in comparison with conventional QM/MM simulations.

Fast implementation of the 1\\rightarrow3 orbital state quantum cloning machine

NASA Astrophysics Data System (ADS)

Lin, Jin-Zhong

2018-05-01

We present a scheme to implement a 1→3 orbital state quantum cloning machine assisted by quantum Zeno dynamics. By constructing shortcuts to adiabatic passage with transitionless quantum driving, we can complete this scheme effectively and quickly in one step. The effects of decoherence, including spontaneous emission and the decay of the cavity, are also discussed. The numerical simulation results show that high fidelity can be obtained and the feasibility analysis indicates that this can also be realized in experiments.

The effect of various quantum mechanically derived partial atomic charges on the bulk properties of chloride-based ionic liquids

NASA Astrophysics Data System (ADS)

Zolghadr, Amin Reza; Ghatee, Mohammad Hadi; Moosavi, Fatemeh

2016-08-01

Partial atomic charges using various quantum mechanical calculations for [Cnmim]Cl (n = 1, 4) ionic liquids (ILs) are obtained and used for development of molecular dynamics simulation (MD) force fields. The isolated ion pairs are optimized using HF, B3LYP, and MP2 methods for electronic structure with 6-311++G(d,p) basis set. Partial atomic charges are assigned to the atomic center with CHELPG and NBO methods. The effect of these sets of partial charges on the static and dynamic properties of ILs is evaluated by performing a series of MD simulations and comparing the essential thermodynamic properties with the available experimental data and available molecular dynamics simulation results. In contrast to the general trends reported for ionic liquids with BF4, PF6, and iodide anions (in which restrained electrostatic potential (RESP) charges are preferred), partial charges derived by B3LYP-NBO method are relatively good in prediction of the structural, dynamical, and thermodynamic energetic properties of the chloride based ILs.

Ab initio quantum direct dynamics simulations of ultrafast photochemistry with Multiconfigurational Ehrenfest approach

NASA Astrophysics Data System (ADS)

Makhov, Dmitry V.; Symonds, Christopher; Fernandez-Alberti, Sebastian; Shalashilin, Dmitrii V.

2017-08-01

The Multiconfigurational Ehrenfest (MCE) method is a quantum dynamics technique which allows treatment of a large number of quantum nuclear degrees of freedom. This paper presents a review of MCE and its recent applications, providing a summary of the formalisms, including its ab initio direct dynamics versions and also giving a summary of recent results. Firstly, we describe the Multiconfigurational Ehrenfest version 2 (MCEv2) method and its applicability to direct dynamics and report new calculations which show that the approach converges to the exact result in model systems with tens of degrees of freedom. Secondly, we review previous ;on the fly; ab initio Multiple Cloning (AIMC-MCE) MCE dynamics results obtained for systems of a similar size, in which the calculations treat every electron and every nucleus of a polyatomic molecule on a fully quantum basis. We also review the Time Dependent Diabatic Basis (TDDB) version of the technique and give an example of its application. We summarise the details of the sampling techniques and interpolations used for calculation of the matrix elements, which make our approach efficient. Future directions of work are outlined.

Linear-algebraic bath transformation for simulating complex open quantum systems

DOE PAGES

Huh, Joonsuk; Mostame, Sarah; Fujita, Takatoshi; ...

2014-12-02

In studying open quantum systems, the environment is often approximated as a collection of non-interacting harmonic oscillators, a configuration also known as the star-bath model. It is also well known that the star-bath can be transformed into a nearest-neighbor interacting chain of oscillators. The chain-bath model has been widely used in renormalization group approaches. The transformation can be obtained by recursion relations or orthogonal polynomials. Based on a simple linear algebraic approach, we propose a bath partition strategy to reduce the system-bath coupling strength. As a result, the non-interacting star-bath is transformed into a set of weakly coupled multiple parallelmore » chains. Furthermore, the transformed bath model allows complex problems to be practically implemented on quantum simulators, and it can also be employed in various numerical simulations of open quantum dynamics.« less

Quantum diffusion of H/D on Ni(111)—A partially adiabatic centroid MD study

NASA Astrophysics Data System (ADS)

Hopkinson, A. R.; Probert, M. I. J.

2018-03-01

We present the results of a theoretical study of H/D diffusion on a Ni(111) surface at a range of temperatures, from 250 K to 75 K. The diffusion is studied using both classical molecular dynamics and the partially adiabatic centroid molecular dynamics method. The calculations are performed with the hydrogen (or deuterium) moving in 3D across a static nickel surface using a novel Fourier interpolated potential energy surface which has been parameterized to density functional theory calculations. The results of the classical simulations are that the calculated diffusion coefficients are far too small and with too large a variation with temperature compared with experiment. By contrast, the quantum simulations are in much better agreement with experiment and show that quantum effects in the diffusion of hydrogen are significant at all temperatures studied. There is also a crossover to a quantum-dominated diffusive regime for temperatures below ˜150 K for hydrogen and ˜85 K for deuterium. The quantum diffusion coefficients are found to accurately reproduce the spread in values with temperature, but with an absolute value that is a little high compared with experiment.

Functional Wigner representation of quantum dynamics of Bose-Einstein condensate

NASA Astrophysics Data System (ADS)

Opanchuk, B.; Drummond, P. D.

2013-04-01

We develop a method of simulating the full quantum field dynamics of multi-mode multi-component Bose-Einstein condensates in a trap. We use the truncated Wigner representation to obtain a probabilistic theory that can be sampled. This method produces c-number stochastic equations which may be solved using conventional stochastic methods. The technique is valid for large mode occupation numbers. We give a detailed derivation of methods of functional Wigner representation appropriate for quantum fields. Our approach describes spatial evolution of spinor components and properly accounts for nonlinear losses. Such techniques are applicable to calculating the leading quantum corrections, including effects such as quantum squeezing, entanglement, EPR correlations, and interactions with engineered nonlinear reservoirs. By using a consistent expansion in the inverse density, we are able to explain an inconsistency in the nonlinear loss equations found by earlier authors.

Quantum Mechanics/Molecular Mechanics Free Energy Maps and Nonadiabatic Simulations for a Photochemical Reaction in DNA: Cyclobutane Thymine Dimer.

PubMed

Mendieta-Moreno, Jesús I; Trabada, Daniel G; Mendieta, Jesús; Lewis, James P; Gómez-Puertas, Paulino; Ortega, José

2016-11-03

The absorption of ultraviolet radiation by DNA may result in harmful genetic lesions that affect DNA replication and transcription, ultimately causing mutations, cancer, and/or cell death. We analyze the most abundant photochemical reaction in DNA, the cyclobutane thymine dimer, using hybrid quantum mechanics/molecular mechanics (QM/MM) techniques and QM/MM nonadiabatic molecular dynamics. We find that, due to its double helix structure, DNA presents a free energy barrier between nonreactive and reactive conformations leading to the photolesion. Moreover, our nonadiabatic simulations show that most of the photoexcited reactive conformations return to standard B-DNA conformations after an ultrafast nonradiative decay to the ground state. This work highlights the importance of dynamical effects (free energy, excited-state dynamics) for the study of photochemical reactions in biological systems.

Entanglement measures in embedding quantum simulators with nuclear spins

NASA Astrophysics Data System (ADS)

Xin, Tao; Pedernales, Julen S.; Solano, Enrique; Long, Gui-Lu

2018-02-01

We implement an embedding quantum simulator (EQS) in nuclear spin systems. The experiment consists of a simulator of up to three qubits, plus a single ancillary qubit, where we are able to efficiently measure the concurrence and the three-tangle of two-qubit and three-qubit systems as they undergo entangling dynamics. The EQS framework allows us to drastically reduce the number of measurements needed for this task, which otherwise would require full-state reconstruction of the qubit system. Our simulator is built of the nuclear spins of four 13C atoms in a molecule of trans-crotonic acid manipulated with NMR techniques.

Nonadiabatic dynamics of photo-induced proton-coupled electron transfer reactions via ring-polymer surface hopping

NASA Astrophysics Data System (ADS)

Shakib, Farnaz; Huo, Pengfei

Photo-induced proton-coupled electron transfer reactions (PCET) are at the heart of energy conversion reactions in photocatalysis. Here, we apply the recently developed ring-polymer surface-hopping (RPSH) approach to simulate the nonadiabatic dynamics of photo-induced PCET. The RPSH method incorporates ring-polymer (RP) quantization of the proton into the fewest-switches surface-hopping (FSSH) approach. Using two diabatic electronic states, corresponding to the electron donor and acceptor states, we model photo-induced PCET with the proton described by a classical isomorphism RP. From the RPSH method, we obtain numerical results that are comparable to those obtained when the proton is treated quantum mechanically. This accuracy stems from incorporating exact quantum statistics, such as proton tunnelling, into approximate quantum dynamics. Additionally, RPSH offers the numerical accuracy along with the computational efficiency. Namely, compared to the FSSH approach in vibronic representation, there is no need to calculate a massive number of vibronic states explicitly. This approach opens up the possibility to accurately and efficiently simulate photo-induced PCET with multiple transferring protons or electrons.

Regular and irregular dynamics of spin-polarized wavepackets in a mesoscopic quantum dot at the edge of topological insulator

NASA Astrophysics Data System (ADS)

Khomitsky, D. V.; Chubanov, A. A.; Konakov, A. A.

2016-12-01

The dynamics of Dirac-Weyl spin-polarized wavepackets driven by a periodic electric field is considered for the electrons in a mesoscopic quantum dot formed at the edge of the two-dimensional HgTe/CdTe topological insulator with Dirac-Weyl massless energy spectra, where the motion of carriers is less sensitive to disorder and impurity potentials. It is observed that the interplay of strongly coupled spin and charge degrees of freedom creates the regimes of irregular dynamics in both coordinate and spin channels. The border between the regular and irregular regimes determined by the strength and frequency of the driving field is found analytically within the quasiclassical approach by means of the Ince-Strutt diagram for the Mathieu equation, and is supported by full quantum-mechanical simulations of the driven dynamics. The investigation of quasienergy spectrum by Floquet approach reveals the presence of non-Poissonian level statistics, which indicates the possibility of chaotic quantum dynamics and corresponds to the areas of parameters for irregular regimes within the quasiclassical approach. We find that the influence of weak disorder leads to partial suppression of the dynamical chaos. Our findings are of interest both for progress in the fundamental field of quantum chaotic dynamics and for further experimental and technological applications of spindependent phenomena in nanostructures based on topological insulators.

Regular and irregular dynamics of spin-polarized wavepackets in a mesoscopic quantum dot at the edge of topological insulator

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

Khomitsky, D. V., E-mail: khomitsky@phys.unn.ru; Chubanov, A. A.; Konakov, A. A.

2016-12-15

The dynamics of Dirac–Weyl spin-polarized wavepackets driven by a periodic electric field is considered for the electrons in a mesoscopic quantum dot formed at the edge of the two-dimensional HgTe/CdTe topological insulator with Dirac–Weyl massless energy spectra, where the motion of carriers is less sensitive to disorder and impurity potentials. It is observed that the interplay of strongly coupled spin and charge degrees of freedom creates the regimes of irregular dynamics in both coordinate and spin channels. The border between the regular and irregular regimes determined by the strength and frequency of the driving field is found analytically within themore » quasiclassical approach by means of the Ince–Strutt diagram for the Mathieu equation, and is supported by full quantum-mechanical simulations of the driven dynamics. The investigation of quasienergy spectrum by Floquet approach reveals the presence of non-Poissonian level statistics, which indicates the possibility of chaotic quantum dynamics and corresponds to the areas of parameters for irregular regimes within the quasiclassical approach. We find that the influence of weak disorder leads to partial suppression of the dynamical chaos. Our findings are of interest both for progress in the fundamental field of quantum chaotic dynamics and for further experimental and technological applications of spindependent phenomena in nanostructures based on topological insulators.« less

Enzymatic Kinetic Isotope Effects from Path-Integral Free Energy Perturbation Theory.

PubMed

Gao, J

2016-01-01

Path-integral free energy perturbation (PI-FEP) theory is presented to directly determine the ratio of quantum mechanical partition functions of different isotopologs in a single simulation. Furthermore, a double averaging strategy is used to carry out the practical simulation, separating the quantum mechanical path integral exactly into two separate calculations, one corresponding to a classical molecular dynamics simulation of the centroid coordinates, and another involving free-particle path-integral sampling over the classical, centroid positions. An integrated centroid path-integral free energy perturbation and umbrella sampling (PI-FEP/UM, or simply, PI-FEP) method along with bisection sampling was summarized, which provides an accurate and fast convergent method for computing kinetic isotope effects for chemical reactions in solution and in enzymes. The PI-FEP method is illustrated by a number of applications, to highlight the computational precision and accuracy, the rule of geometrical mean in kinetic isotope effects, enhanced nuclear quantum effects in enzyme catalysis, and protein dynamics on temperature dependence of kinetic isotope effects. © 2016 Elsevier Inc. All rights reserved.

Carbinolamine Formation and Dehydration in a DNA Repair Enzyme Active Site

PubMed Central

Dodson, M. L.; Walker, Ross C.; Lloyd, R. Stephen

2012-01-01

In order to suggest detailed mechanistic hypotheses for the formation and dehydration of a key carbinolamine intermediate in the T4 pyrimidine dimer glycosylase (T4PDG) reaction, we have investigated these reactions using steered molecular dynamics with a coupled quantum mechanics–molecular mechanics potential (QM/MM). We carried out simulations of DNA abasic site carbinolamine formation with and without a water molecule restrained to remain within the active site quantum region. We recovered potentials of mean force (PMF) from thirty replicate reaction trajectories using Jarzynski averaging. We demonstrated feasible pathways involving water, as well as those independent of water participation. The water–independent enzyme–catalyzed reaction had a bias–corrected Jarzynski–average barrier height of approximately for the carbinolamine formation reaction and ) for the reverse reaction at this level of representation. When the proton transfer was facilitated with an intrinsic quantum water, the barrier height was approximately in the forward (formation) reaction and for the reverse. In addition, two modes of unsteered (free dynamics) carbinolamine dehydration were observed: in one, the quantum water participated as an intermediate proton transfer species, and in the other, the active site protonated glutamate hydrogen was directly transferred to the carbinolamine oxygen. Water–independent unforced proton transfer from the protonated active site glutamate carboxyl to the unprotonated N–terminal amine was also observed. In summary, complex proton transfer events, some involving water intermediates, were studied in QM/MM simulations of T4PDG bound to a DNA abasic site. Imine carbinolamine formation was characterized using steered QM/MM molecular dynamics. Dehydration of the carbinolamine intermediate to form the final imine product was observed in free, unsteered, QM/MM dynamics simulations, as was unforced acid-base transfer between the active site carboxylate and the N–terminal amine. PMID:22384015

Coherent Dynamics of Open Quantum System in the Presence of Majorana Fermions

NASA Astrophysics Data System (ADS)

Assuncao, Maryzaura O.; Diniz, Ginetom S.; Vernek, Edson; Souza, Fabricio M.

In recent years the research on quantum coherent dynamics of open systems has attracted great attention due to its relevance for future implementation of quantum computers. In the present study we apply the Kadanoff-Baym formalism to simulate the population dynamics of a double-dot molecular system attached to both a superconductor and fermionic reservoirs. We solve both analytically and numerically a set of coupled differential equations that account for crossed Andreev reflection (CAR), intramolecular hopping and tunneling. We pay particular attention on how Majorana bound states can affect the population dynamics of the molecule. We investigate on how initial state configuration affects the dynamics. For instance, if one dot is occupied and the other one is empty, the dynamics is dictated by the inter dot tunneling. On the other hand, for initially empty dots, the CAR dominates. We also investigate how the source and drain currents evolve in time. This work was supporte by FAPEMIG, CNPq and CAPES.

Quantum dynamics simulations in an ultraslow bath using hierarchy of stochastic Schrödinger equations

NASA Astrophysics Data System (ADS)

Ke, Yaling; Zhao, Yi

2018-04-01

The hierarchy of stochastic Schrödinger equation, previously developed under the unpolarised initial bath states, is extended in this paper for open quantum dynamics under polarised initial bath conditions. The method is proved to be a powerful tool in investigating quantum dynamics exposed to an ultraslow Ohmic bath, as in this case the hierarchical truncation level and the random sampling number can be kept at a relatively small extent. By systematically increasing the system-bath coupling strength, the symmetric Ohmic spin-boson dynamics is investigated at finite temperature, with a very small cut-off frequency. It is confirmed that the slow bath makes the system dynamics extremely sensitive to the initial bath conditions. The localisation tendency is stronger in the polarised initial bath conditions. Besides, the oscillatory coherent dynamics persists even when the system-bath coupling is very strong, in correspondence with what is found recently in the deep sub-Ohmic bath, where also the low-frequency modes dominate.

Open-system dynamics of entanglement:a key issues review

NASA Astrophysics Data System (ADS)

Aolita, Leandro; de Melo, Fernando; Davidovich, Luiz

2015-04-01

One of the greatest challenges in the fields of quantum information processing and quantum technologies is the detailed coherent control over each and every constituent of quantum systems with an ever increasing number of particles. Within this endeavor, harnessing of many-body entanglement against the detrimental effects of the environment is a major pressing issue. Besides being an important concept from a fundamental standpoint, entanglement has been recognized as a crucial resource for quantum speed-ups or performance enhancements over classical methods. Understanding and controlling many-body entanglement in open systems may have strong implications in quantum computing, quantum simulations of many-body systems, secure quantum communication or cryptography, quantum metrology, our understanding of the quantum-to-classical transition, and other important questions of quantum foundations. In this paper we present an overview of recent theoretical and experimental efforts to underpin the dynamics of entanglement under the influence of noise. Entanglement is thus taken as a dynamic quantity on its own, and we survey how it evolves due to the unavoidable interaction of the entangled system with its surroundings. We analyze several scenarios, corresponding to different families of states and environments, which render a very rich diversity of dynamical behaviors. In contrast to single-particle quantities, like populations and coherences, which typically vanish only asymptotically in time, entanglement may disappear at a finite time. In addition, important classes of entanglement display an exponential decay with the number of particles when subject to local noise, which poses yet another threat to the already-challenging scaling of quantum technologies. Other classes, however, turn out to be extremely robust against local noise. Theoretical results and recent experiments regarding the difference between local and global decoherence are summarized. Control and robustness-enhancement techniques, scaling laws, statistical and geometrical aspects of multipartite-entanglement decay are also reviewed; all in order to give a broad picture of entanglement dynamics in open quantum systems addressed to both theorists and experimentalists inside and outside the field of quantum information.

Open-system dynamics of entanglement: a key issues review.

PubMed

Aolita, Leandro; de Melo, Fernando; Davidovich, Luiz

2015-04-01

One of the greatest challenges in the fields of quantum information processing and quantum technologies is the detailed coherent control over each and every constituent of quantum systems with an ever increasing number of particles. Within this endeavor, harnessing of many-body entanglement against the detrimental effects of the environment is a major pressing issue. Besides being an important concept from a fundamental standpoint, entanglement has been recognized as a crucial resource for quantum speed-ups or performance enhancements over classical methods. Understanding and controlling many-body entanglement in open systems may have strong implications in quantum computing, quantum simulations of many-body systems, secure quantum communication or cryptography, quantum metrology, our understanding of the quantum-to-classical transition, and other important questions of quantum foundations.In this paper we present an overview of recent theoretical and experimental efforts to underpin the dynamics of entanglement under the influence of noise. Entanglement is thus taken as a dynamic quantity on its own, and we survey how it evolves due to the unavoidable interaction of the entangled system with its surroundings. We analyze several scenarios, corresponding to different families of states and environments, which render a very rich diversity of dynamical behaviors.In contrast to single-particle quantities, like populations and coherences, which typically vanish only asymptotically in time, entanglement may disappear at a finite time. In addition, important classes of entanglement display an exponential decay with the number of particles when subject to local noise, which poses yet another threat to the already-challenging scaling of quantum technologies. Other classes, however, turn out to be extremely robust against local noise. Theoretical results and recent experiments regarding the difference between local and global decoherence are summarized. Control and robustness-enhancement techniques, scaling laws, statistical and geometrical aspects of multipartite-entanglement decay are also reviewed; all in order to give a broad picture of entanglement dynamics in open quantum systems addressed to both theorists and experimentalists inside and outside the field of quantum information.

Counter-diabatic driving for Dirac dynamics

NASA Astrophysics Data System (ADS)

Fan, Qi-Zhen; Cheng, Xiao-Hang; Chen, Xi

2018-03-01

In this paper, we investigate the fast quantum control of Dirac equation dynamics by counter-diabatic driving, sharing the concept of shortcut to adiabaticity. We systematically calculate the counter-diabatic terms in different Dirac systems, like graphene and trapped ions. Specially, the fast and robust population inversion processes are achieved in Dirac system, taking into account the quantum simulation with trapped ions. In addition, the population transfer between two bands can be suppressed by counter-diabatic driving in graphene system, which might have potential applications in opt-electric devices.

Dynamic microscale temperature gradient in a gold nanorod solution measured by diffraction-limited nanothermometry

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

Li, Chengmingyue; Gan, Xiaosong; Li, Xiangping

2015-09-21

We quantify the dynamic microscale temperature gradient in a gold nanorod solution using quantum-dot-based microscopic fluorescence nanothermometry. By incorporating CdSe quantum dots into the solution as a nanothermometer, precise temperature mapping with diffraction-limited spatial resolution and sub-degree temperature resolution is achieved. The acquired data on heat generation and dissipation show an excellent agreement with theoretical simulations. This work reveals an effective approach for noninvasive temperature regulation with localized nanoheaters in microfluidic environment.

Nuclear Quantum Effects in Water and Aqueous Systems: Experiment, Theory, and Current Challenges

DOE PAGES

Ceriotti, Michele; Fang, Wei; Kusalik, Peter G.; ...

2016-04-06

Nuclear quantum effects influence the structure and dynamics of hydrogen bonded systems, such as water, which impacts their observed properties with widely varying magnitudes. This review highlights the recent significant developments in the experiment, theory and simulation of nuclear quantum effects in water. Novel experimental techniques, such as deep inelastic neutron scattering, now provide a detailed view of the role of nuclear quantum effects in water’s properties. These have been combined with theoretical developments such as the introduction of the competing quantum effects principle that allows the subtle interplay of water’s quantum effects and their manifestation in experimental observables tomore » be explained. We discuss how this principle has recently been used to explain the apparent dichotomy in water’s isotope effects, which can range from very large to almost nonexistent depending on the property and conditions. We then review the latest major developments in simulation algorithms and theory that have enabled the efficient inclusion of nuclear quantum effects in molecular simulations, permitting their combination with on-the-fly evaluation of the potential energy surface using electronic structure theory. Finally, we identify current challenges and future opportunities in the area.« less

Quantum spin chains with multiple dynamics

NASA Astrophysics Data System (ADS)

Chen, Xiao; Fradkin, Eduardo; Witczak-Krempa, William

2017-11-01

Many-body systems with multiple emergent time scales arise in various contexts, including classical critical systems, correlated quantum materials, and ultracold atoms. We investigate such nontrivial quantum dynamics in a different setting: a spin-1 bilinear-biquadratic chain. It has a solvable entangled ground state, but a gapless excitation spectrum that is poorly understood. By using large-scale density matrix renormalization group simulations, we find that the lowest excitations have a dynamical exponent z that varies from 2 to 3.2 as we vary a coupling in the Hamiltonian. We find an additional gapless mode with a continuously varying exponent 2 ≤z <2.7 , which establishes the presence of multiple dynamics. In order to explain these striking properties, we construct a continuum wave function for the ground state, which correctly describes the correlations and entanglement properties. We also give a continuum parent Hamiltonian, but show that additional ingredients are needed to capture the excitations of the chain. By using an exact mapping to the nonequilibrium dynamics of a classical spin chain, we find that the large dynamical exponent is due to subdiffusive spin motion. Finally, we discuss the connections to other spin chains and to a family of quantum critical models in two dimensions.

Simulation and understanding of atomic and molecular quantum crystals

NASA Astrophysics Data System (ADS)

Cazorla, Claudio; Boronat, Jordi

2017-07-01

Quantum crystals abound in the whole range of solid-state species. Below a certain threshold temperature the physical behavior of rare gases (He 4 and Ne), molecular solids (H2 and CH4 ), and some ionic (LiH), covalent (graphite), and metallic (Li) crystals can be explained only in terms of quantum nuclear effects (QNE). A detailed comprehension of the nature of quantum solids is critical for achieving progress in a number of fundamental and applied scientific fields such as planetary sciences, hydrogen storage, nuclear energy, quantum computing, and nanoelectronics. This review describes the current physical understanding of quantum crystals formed by atoms and small molecules, as well as the wide palette of simulation techniques that are used to investigate them. Relevant aspects in these materials such as phase transformations, structural properties, elasticity, crystalline defects, and the effects of reduced dimensionality are discussed thoroughly. An introduction to quantum Monte Carlo techniques, which in the present context are the simulation methods of choice, and other quantum simulation approaches (e.g., path-integral molecular dynamics and quantum thermal baths) is provided. The overarching objective of this article is twofold: first, to clarify in which crystals and physical situations the disregard of QNE may incur in important bias and erroneous interpretations. And second, to promote the study and appreciation of QNE, a topic that traditionally has been treated in the context of condensed matter physics, within the broad and interdisciplinary areas of materials science.

Strong Coupling and Entanglement of Quantum Emitters Embedded in a Nanoantenna-Enhanced Plasmonic Cavity

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

Hensen, Matthias; Heilpern, Tal; Gray, Stephen K.

Establishing strong coupling between spatially separated and thus selectively addressable quantum emitters is a key ingredient to complex quantum optical schemes in future technologies. Insofar as many plasmonic nanostructures are concerned, however, the energy transfer and mutual interaction strength between distant quantum emitters can fail to provide strong coupling. Here, based on mode hybridization, the longevity and waveguide character of an elliptical plasmon cavity are combined with intense and highly localized field modes of suitably designed nanoantennas. Based on FDTD simulations a quantum emitter-plasmon coupling strength hg = 16.7 meV is reached while simultaneously keeping a small plasmon resonance linemore » width h gamma(s) = 33 meV. This facilitates strong coupling, and quantum dynamical simulations reveal an oscillatory exchange of excited state population arid a notable degree of entanglement between the quantum emitters spatially separated by 1.8 mu m, i.e., about twice the operating wavelength.« less

A general transfer-function approach to noise filtering in open-loop quantum control

NASA Astrophysics Data System (ADS)

Viola, Lorenza

2015-03-01

Hamiltonian engineering via unitary open-loop quantum control provides a versatile and experimentally validated framework for manipulating a broad class of non-Markovian open quantum systems of interest, with applications ranging from dynamical decoupling and dynamically corrected quantum gates, to noise spectroscopy and quantum simulation. In this context, transfer-function techniques directly motivated by control engineering have proved invaluable for obtaining a transparent picture of the controlled dynamics in the frequency domain and for quantitatively analyzing performance. In this talk, I will show how to identify a computationally tractable set of ``fundamental filter functions,'' out of which arbitrary filter functions may be assembled up to arbitrary high order in principle. Besides avoiding the infinite recursive hierarchy of filter functions that arises in general control scenarios, this fundamental set suffices to characterize the error suppression capabilities of the control protocol in both the time and frequency domain. I will show, in particular, how the resulting notion of ``filtering order'' reveals conceptually distinct, albeit complementary, features of the controlled dynamics as compared to the ``cancellation order,'' traditionally defined in the Magnus sense. Implications for current quantum control experiments will be discussed. Work supported by the U.S. Army Research Office under Contract No. W911NF-14-1-0682.

A unified stochastic formulation of dissipative quantum dynamics. I. Generalized hierarchical equations

NASA Astrophysics Data System (ADS)

Hsieh, Chang-Yu; Cao, Jianshu

2018-01-01

We extend a standard stochastic theory to study open quantum systems coupled to a generic quantum environment. We exemplify the general framework by studying a two-level quantum system coupled bilinearly to the three fundamental classes of non-interacting particles: bosons, fermions, and spins. In this unified stochastic approach, the generalized stochastic Liouville equation (SLE) formally captures the exact quantum dissipations when noise variables with appropriate statistics for different bath models are applied. Anharmonic effects of a non-Gaussian bath are precisely encoded in the bath multi-time correlation functions that noise variables have to satisfy. Starting from the SLE, we devise a family of generalized hierarchical equations by averaging out the noise variables and expand bath multi-time correlation functions in a complete basis of orthonormal functions. The general hierarchical equations constitute systems of linear equations that provide numerically exact simulations of quantum dynamics. For bosonic bath models, our general hierarchical equation of motion reduces exactly to an extended version of hierarchical equation of motion which allows efficient simulation for arbitrary spectral densities and temperature regimes. Similar efficiency and flexibility can be achieved for the fermionic bath models within our formalism. The spin bath models can be simulated with two complementary approaches in the present formalism. (I) They can be viewed as an example of non-Gaussian bath models and be directly handled with the general hierarchical equation approach given their multi-time correlation functions. (II) Alternatively, each bath spin can be first mapped onto a pair of fermions and be treated as fermionic environments within the present formalism.

Dynamics of Quantum Adiabatic Evolution Algorithm for Number Partitioning

NASA Technical Reports Server (NTRS)

Smelyanskiy, V. N.; Toussaint, U. V.; Timucin, D. A.

2002-01-01

We have developed a general technique to study the dynamics of the quantum adiabatic evolution algorithm applied to random combinatorial optimization problems in the asymptotic limit of large problem size n. We use as an example the NP-complete Number Partitioning problem and map the algorithm dynamics to that of an auxiliary quantum spin glass system with the slowly varying Hamiltonian. We use a Green function method to obtain the adiabatic eigenstates and the minimum excitation gap. g min, = O(n 2(exp -n/2), corresponding to the exponential complexity of the algorithm for Number Partitioning. The key element of the analysis is the conditional energy distribution computed for the set of all spin configurations generated from a given (ancestor) configuration by simultaneous flipping of a fixed number of spins. For the problem in question this distribution is shown to depend on the ancestor spin configuration only via a certain parameter related to 'the energy of the configuration. As the result, the algorithm dynamics can be described in terms of one-dimensional quantum diffusion in the energy space. This effect provides a general limitation of a quantum adiabatic computation in random optimization problems. Analytical results are in agreement with the numerical simulation of the algorithm.

Dynamics of Quantum Adiabatic Evolution Algorithm for Number Partitioning

NASA Technical Reports Server (NTRS)

Smelyanskiy, Vadius; vonToussaint, Udo V.; Timucin, Dogan A.; Clancy, Daniel (Technical Monitor)

2002-01-01

We have developed a general technique to study the dynamics of the quantum adiabatic evolution algorithm applied to random combinatorial optimization problems in the asymptotic limit of large problem size n. We use as an example the NP-complete Number Partitioning problem and map the algorithm dynamics to that of an auxiliary quantum spin glass system with the slowly varying Hamiltonian. We use a Green function method to obtain the adiabatic eigenstates and the minimum exitation gap, gmin = O(n2(sup -n/2)), corresponding to the exponential complexity of the algorithm for Number Partitioning. The key element of the analysis is the conditional energy distribution computed for the set of all spin configurations generated from a given (ancestor) configuration by simultaneous flipping of a fixed number of spins. For the problem in question this distribution is shown to depend on the ancestor spin configuration only via a certain parameter related to the energy of the configuration. As the result, the algorithm dynamics can be described in terms of one-dimensional quantum diffusion in the energy space. This effect provides a general limitation of a quantum adiabatic computation in random optimization problems. Analytical results are in agreement with the numerical simulation of the algorithm.

Novel Image Encryption based on Quantum Walks

PubMed Central

Yang, Yu-Guang; Pan, Qing-Xiang; Sun, Si-Jia; Xu, Peng

2015-01-01

Quantum computation has achieved a tremendous success during the last decades. In this paper, we investigate the potential application of a famous quantum computation model, i.e., quantum walks (QW) in image encryption. It is found that QW can serve as an excellent key generator thanks to its inherent nonlinear chaotic dynamic behavior. Furthermore, we construct a novel QW-based image encryption algorithm. Simulations and performance comparisons show that the proposal is secure enough for image encryption and outperforms prior works. It also opens the door towards introducing quantum computation into image encryption and promotes the convergence between quantum computation and image processing. PMID:25586889

Nicholas Metropolis Award for Outstanding Doctoral Thesis Work in Computational Physics: Quantum many-body physics of ultracold molecules in optical lattices: models and simulation methods

NASA Astrophysics Data System (ADS)

Wall, Michael

2014-03-01

Experimental progress in generating and manipulating synthetic quantum systems, such as ultracold atoms and molecules in optical lattices, has revolutionized our understanding of quantum many-body phenomena and posed new challenges for modern numerical techniques. Ultracold molecules, in particular, feature long-range dipole-dipole interactions and a complex and selectively accessible internal structure of rotational and hyperfine states, leading to many-body models with long range interactions and many internal degrees of freedom. Additionally, the many-body physics of ultracold molecules is often probed far from equilibrium, and so algorithms which simulate quantum many-body dynamics are essential. Numerical methods which are to have significant impact in the design and understanding of such synthetic quantum materials must be able to adapt to a variety of different interactions, physical degrees of freedom, and out-of-equilibrium dynamical protocols. Matrix product state (MPS)-based methods, such as the density-matrix renormalization group (DMRG), have become the de facto standard for strongly interacting low-dimensional systems. Moreover, the flexibility of MPS-based methods makes them ideally suited both to generic, open source implementation as well as to studies of the quantum many-body dynamics of ultracold molecules. After introducing MPSs and variational algorithms using MPSs generally, I will discuss my own research using MPSs for many-body dynamics of long-range interacting systems. In addition, I will describe two open source implementations of MPS-based algorithms in which I was involved, as well as educational materials designed to help undergraduates and graduates perform research in computational quantum many-body physics using a variety of numerical methods including exact diagonalization and static and dynamic variational MPS methods. Finally, I will mention present research on ultracold molecules in optical lattices, such as the exploration of many-body physics with polyatomic molecules, and the next generation of open source matrix product state codes. This work was performed in the research group of Prof. Lincoln D. Carr.

Bloch oscillations in the absence of a lattice

NASA Astrophysics Data System (ADS)

Meinert, Florian; Knap, Michael; Kirilov, Emil; Jag-Lauber, Katharina; Zvonarev, Mikhail B.; Demler, Eugene; Nägerl, Hanns-Christoph

2017-06-01

The interplay of strong quantum correlations and far-from-equilibrium conditions can give rise to striking dynamical phenomena. We experimentally investigated the quantum motion of an impurity atom immersed in a strongly interacting one-dimensional Bose liquid and subject to an external force. We found that the momentum distribution of the impurity exhibits characteristic Bragg reflections at the edge of an emergent Brillouin zone. Although Bragg reflections are typically associated with lattice structures, in our strongly correlated quantum liquid they result from the interplay of short-range crystalline order and kinematic constraints on the many-body scattering processes in the one-dimensional system. As a consequence, the impurity exhibits periodic dynamics, reminiscent of Bloch oscillations, although the quantum liquid is translationally invariant. Our observations are supported by large-scale numerical simulations.

On the mode-coupling treatment of collective density fluctuations for quantum liquids: para-hydrogen and normal liquid helium.

PubMed

Kletenik-Edelman, Orly; Reichman, David R; Rabani, Eran

2011-01-28

A novel quantum mode coupling theory combined with a kinetic approach is developed for the description of collective density fluctuations in quantum liquids characterized by Boltzmann statistics. Three mode-coupling approximations are presented and applied to study the dynamic response of para-hydrogen near the triple point and normal liquid helium above the λ-transition. The theory is compared with experimental results and to the exact imaginary time data generated by path integral Monte Carlo simulations. While for liquid para-hydrogen the combination of kinetic and quantum mode-coupling theory provides semi-quantitative results for both short and long time dynamics, it fails for normal liquid helium. A discussion of this failure based on the ideal gas limit is presented.

Investigation of monolithic passively mode-locked quantum dot lasers with extremely low repetition frequency.

PubMed

Xu, Tianhong; Cao, Juncheng; Montrosset, Ivo

2015-01-01

The dynamical regimes and performance optimization of quantum dot monolithic passively mode-locked lasers with extremely low repetition rate are investigated using the numerical method. A modified multisection delayed differential equation model is proposed to accomplish simulations of both two-section and three-section passively mode-locked lasers with long cavity. According to the numerical simulations, it is shown that fundamental and harmonic mode-locking regimes can be multistable over a wide current range. These dynamic regimes are studied, and the reasons for their existence are explained. In addition, we demonstrate that fundamental pulses with higher peak power can be achieved when the laser is designed to work in a region with smaller differential gain.

Functional Wigner representation of quantum dynamics of Bose-Einstein condensate

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

Opanchuk, B.; Drummond, P. D.

2013-04-15

We develop a method of simulating the full quantum field dynamics of multi-mode multi-component Bose-Einstein condensates in a trap. We use the truncated Wigner representation to obtain a probabilistic theory that can be sampled. This method produces c-number stochastic equations which may be solved using conventional stochastic methods. The technique is valid for large mode occupation numbers. We give a detailed derivation of methods of functional Wigner representation appropriate for quantum fields. Our approach describes spatial evolution of spinor components and properly accounts for nonlinear losses. Such techniques are applicable to calculating the leading quantum corrections, including effects such asmore » quantum squeezing, entanglement, EPR correlations, and interactions with engineered nonlinear reservoirs. By using a consistent expansion in the inverse density, we are able to explain an inconsistency in the nonlinear loss equations found by earlier authors.« less

Andreev reflection, a tool to investigate vortex dynamics and quantum turbulence in 3He-B.

PubMed

Fisher, Shaun Neil; Jackson, Martin James; Sergeev, Yuri A; Tsepelin, Viktor

2014-03-25

Andreev reflection of quasiparticle excitations provides a sensitive and passive probe of flow in superfluid (3)He-B. It is particularly useful for studying complex flows generated by vortex rings and vortex tangles (quantum turbulence). We describe the reflection process and discuss the results of numerical simulations of Andreev reflection from vortex rings and from quantum turbulence. We present measurements of vortices generated by a vibrating grid resonator at very low temperatures. The Andreev reflection is measured using an array of vibrating wire sensors. At low grid velocities, ballistic vortex rings are produced. At higher grid velocities, the rings collide and reconnect to produce quantum turbulence. We discuss spatial correlations of the fluctuating vortex signals measured by the different sensor wires. These reveal detailed information about the formation of quantum turbulence and about the underlying vortex dynamics.

Andreev reflection, a tool to investigate vortex dynamics and quantum turbulence in 3He-B

PubMed Central

Fisher, Shaun Neil; Jackson, Martin James; Sergeev, Yuri A.; Tsepelin, Viktor

2014-01-01

Andreev reflection of quasiparticle excitations provides a sensitive and passive probe of flow in superfluid 3He-B. It is particularly useful for studying complex flows generated by vortex rings and vortex tangles (quantum turbulence). We describe the reflection process and discuss the results of numerical simulations of Andreev reflection from vortex rings and from quantum turbulence. We present measurements of vortices generated by a vibrating grid resonator at very low temperatures. The Andreev reflection is measured using an array of vibrating wire sensors. At low grid velocities, ballistic vortex rings are produced. At higher grid velocities, the rings collide and reconnect to produce quantum turbulence. We discuss spatial correlations of the fluctuating vortex signals measured by the different sensor wires. These reveal detailed information about the formation of quantum turbulence and about the underlying vortex dynamics. PMID:24704872

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.

Zero point energy leakage in condensed phase dynamics: An assessment of quantum simulation methods for liquid water

NASA Astrophysics Data System (ADS)

Habershon, Scott; Manolopoulos, David E.

2009-12-01

The approximate quantum mechanical ring polymer molecular dynamics (RPMD) and linearized semiclassical initial value representation (LSC-IVR) methods are compared and contrasted in a study of the dynamics of the flexible q-TIP4P/F water model at room temperature. For this water model, a RPMD simulation gives a diffusion coefficient that is only a few percent larger than the classical diffusion coefficient, whereas a LSC-IVR simulation gives a diffusion coefficient that is three times larger. We attribute this discrepancy to the unphysical leakage of initially quantized zero point energy (ZPE) from the intramolecular to the intermolecular modes of the liquid as the LSC-IVR simulation progresses. In spite of this problem, which is avoided by construction in RPMD, the LSC-IVR may still provide a useful approximation to certain short-time dynamical properties which are not so strongly affected by the ZPE leakage. We illustrate this with an application to the liquid water dipole absorption spectrum, for which the RPMD approximation breaks down at frequencies in the O-H stretching region owing to contamination from the internal modes of the ring polymer. The LSC-IVR does not suffer from this difficulty and it appears to provide quite a promising way to calculate condensed phase vibrational spectra.

Zero point energy leakage in condensed phase dynamics: an assessment of quantum simulation methods for liquid water.

PubMed

Habershon, Scott; Manolopoulos, David E

2009-12-28

The approximate quantum mechanical ring polymer molecular dynamics (RPMD) and linearized semiclassical initial value representation (LSC-IVR) methods are compared and contrasted in a study of the dynamics of the flexible q-TIP4P/F water model at room temperature. For this water model, a RPMD simulation gives a diffusion coefficient that is only a few percent larger than the classical diffusion coefficient, whereas a LSC-IVR simulation gives a diffusion coefficient that is three times larger. We attribute this discrepancy to the unphysical leakage of initially quantized zero point energy (ZPE) from the intramolecular to the intermolecular modes of the liquid as the LSC-IVR simulation progresses. In spite of this problem, which is avoided by construction in RPMD, the LSC-IVR may still provide a useful approximation to certain short-time dynamical properties which are not so strongly affected by the ZPE leakage. We illustrate this with an application to the liquid water dipole absorption spectrum, for which the RPMD approximation breaks down at frequencies in the O-H stretching region owing to contamination from the internal modes of the ring polymer. The LSC-IVR does not suffer from this difficulty and it appears to provide quite a promising way to calculate condensed phase vibrational spectra.

Quantum Kibble-Zurek Mechanism in a Spin-1 Bose-Einstein Condensate

NASA Astrophysics Data System (ADS)

Anquez, M.; Robbins, B. A.; Bharath, H. M.; Boguslawski, M.; Hoang, T. M.; Chapman, M. S.

2016-04-01

The dynamics of a quantum phase transition are explored using slow quenches from the polar to the broken-axisymmetry phases in a small spin-1 ferromagnetic Bose-Einstein condensate. Measurements of the evolution of the spin populations reveal a power-law scaling of the temporal onset of excitations versus quench speed as predicted from quantum extensions of the Kibble-Zurek mechanism. The satisfactory agreement of the measured scaling exponent with the analytical theory and numerical simulations provides experimental confirmation of the quantum Kibble-Zurek model.

Modes of asymmetry: The application of harmonic analysis to symmetric quantum dynamics and quantum reference frames

NASA Astrophysics Data System (ADS)

Marvian, Iman; Spekkens, Robert W.

2014-12-01

Finding the consequences of symmetry for open-system quantum dynamics is a problem with broad applications, including describing thermal relaxation, deriving quantum limits on the performance of amplifiers, and exploring quantum metrology in the presence of noise. The symmetry of the dynamics may reflect a symmetry of the fundamental laws of nature or a symmetry of a low-energy effective theory, or it may describe a practical restriction such as the lack of a reference frame. In this paper, we apply some tools of harmonic analysis together with ideas from quantum information theory to this problem. The central idea is to study the decomposition of quantum operations—in particular, states, measurements, and channels—into different modes, which we call modes of asymmetry. Under symmetric processing, a given mode of the input is mapped to the corresponding mode of the output, implying that one can only generate a given output if the input contains all of the necessary modes. By defining monotones that quantify the asymmetry in a particular mode, we also derive quantitative constraints on the resources of asymmetry that are required to simulate a given asymmetric operation. We present applications of our results for deriving bounds on the probability of success in nondeterministic state transitions, such as quantum amplification, and a simplified formalism for studying the degradation of quantum reference frames.

Carbon Nanotube Based Molecular Electronics and Motors: A View from Classical and Quantum Dynamics Simulations

NASA Technical Reports Server (NTRS)

Srivastava, Deepak; Saini, Subhash (Technical Monitor)

1998-01-01

The tubular forms of fullerenes popularly known as carbon nanotubes are experimentally produced as single-, multiwall, and rope configurations. The nanotubes and nanoropes have shown to exhibit unusual mechanical and electronic properties. The single wall nanotubes exhibit both semiconducting and metallic behavior. In short undefected lengths they are the known strongest fibers which are unbreakable even when bent in half. Grown in ropes their tensile strength is approximately 100 times greater than steel at only one sixth the weight. Employing large scale classical and quantum molecular dynamics simulations we will explore the use of carbon nanotubes and carbon nanotube junctions in 2-, 3-, and 4-point molecular electronic device components, dynamic strength characterization for compressive, bending and torsional strains, and chemical functionalization for possible use in a nanoscale molecular motor. The above is an unclassified material produced for non-competitive basic research in the nanotechnology area.

Quantum Chemical Molecular Dynamics Simulations of 1,3-Dichloropropene Combustion.

PubMed

Ahubelem, Nwakamma; Shah, Kalpit; Moghtaderi, Behdad; Page, Alister J

2015-09-03

Oxidative decomposition of 1,3-dichloropropene was investigated using quantum chemical molecular dynamics (QM/MD) at 1500 and 3000 K. Thermal oxidation of 1,3-dichloropropene was initiated by (1) abstraction of allylic H/Cl by O2 and (2) intra-annular C-Cl bond scission and elimination of allylic Cl. A kinetic analysis shows that (2) is the more dominant initiation pathway, in agreement with QM/MD results. These QM/MD simulations reveal new routes to the formation of major products (H2O, CO, HCl, CO2), which are propagated primarily by the chloroperoxy (ClO2), OH, and 1,3-dichloropropene derived radicals. In particular, intra-annular C-C/C-H bond dissociation reactions of intermediate aldehydes/ketones are shown to play a dominant role in the formation of CO and CO2. Our simulations demonstrate that both combustion temperature and radical concentration can influence the product yield, however not the combustion mechanism.

Comparison of Chain Conformation of Poly(vinyl alcohol) in Solutions and Melts from Quantum Chemistry Based Molecular Dynamics Simulations

NASA Technical Reports Server (NTRS)

Jaffe, Richard; Han, Jie; Matsuda, Tsunetoshi; Yoon, Do; Langhoff, Stephen R. (Technical Monitor)

1997-01-01

Confirmations of 2,4-dihydroxypentane (DHP), a model molecule for poly(vinyl alcohol), have been studied by quantum chemistry (QC) calculations and molecular dynamics (MD) simulations. QC calculations at the 6-311G MP2 level show the meso tt conformer to be lowest in energy followed by the racemic tg, due to intramolecular hydrogen bond between the hydroxy groups. The Dreiding force field has been modified to reproduce the QC conformer energies for DHP. MD simulations using this force field have been carried out for DHP molecules in the gas phase, melt, and CHCl3 and water solutions. Extensive intramolecular hydrogen bonding is observed for the gas phase and CHCl3 solution, but not for the melt or aqueous solution, Such a condensed phase effect due to intermolecular interactions results in a drastic change in chain conformations, in agreement with experiments.

Internal force corrections with machine learning for quantum mechanics/molecular mechanics simulations.

PubMed

Wu, Jingheng; Shen, Lin; Yang, Weitao

2017-10-28

Ab initio quantum mechanics/molecular mechanics (QM/MM) molecular dynamics simulation is a useful tool to calculate thermodynamic properties such as potential of mean force for chemical reactions but intensely time consuming. In this paper, we developed a new method using the internal force correction for low-level semiempirical QM/MM molecular dynamics samplings with a predefined reaction coordinate. As a correction term, the internal force was predicted with a machine learning scheme, which provides a sophisticated force field, and added to the atomic forces on the reaction coordinate related atoms at each integration step. We applied this method to two reactions in aqueous solution and reproduced potentials of mean force at the ab initio QM/MM level. The saving in computational cost is about 2 orders of magnitude. The present work reveals great potentials for machine learning in QM/MM simulations to study complex chemical processes.

Measuring out-of-time-order correlations and multiple quantum spectra in a trapped-ion quantum magnet

NASA Astrophysics Data System (ADS)

Gärttner, Martin; Bohnet, Justin G.; Safavi-Naini, Arghavan; Wall, Michael L.; Bollinger, John J.; Rey, Ana Maria

2017-08-01

Controllable arrays of ions and ultracold atoms can simulate complex many-body phenomena and may provide insights into unsolved problems in modern science. To this end, experimentally feasible protocols for quantifying the buildup of quantum correlations and coherence are needed, as performing full state tomography does not scale favourably with the number of particles. Here we develop and experimentally demonstrate such a protocol, which uses time reversal of the many-body dynamics to measure out-of-time-order correlation functions (OTOCs) in a long-range Ising spin quantum simulator with more than 100 ions in a Penning trap. By measuring a family of OTOCs as a function of a tunable parameter we obtain fine-grained information about the state of the system encoded in the multiple quantum coherence spectrum, extract the quantum state purity, and demonstrate the buildup of up to 8-body correlations. Future applications of this protocol could enable studies of many-body localization, quantum phase transitions, and tests of the holographic duality between quantum and gravitational systems.

Effects of stochastic noise on dynamical decoupling procedures

NASA Astrophysics Data System (ADS)

Bernád, J. Z.; Frydrych, H.

2014-06-01

Dynamical decoupling is an important tool to counter decoherence and dissipation effects in quantum systems originating from environmental interactions. It has been used successfully in many experiments; however, there is still a gap between fidelity improvements achieved in practice compared to theoretical predictions. We propose a model for imperfect dynamical decoupling based on a stochastic Ito differential equation which could explain the observed gap. We discuss the impact of our model on the time evolution of various quantum systems in finite- and infinite-dimensional Hilbert spaces. Analytical results are given for the limit of continuous control, whereas we present numerical simulations and upper bounds for the case of finite control.

Photoinduced Single- and Multiple-Electron Dynamics Processes Enhanced by Quantum Confinement in Lead Halide Perovskite Quantum Dots

DOE PAGES

Vogel, Dayton J.; Kryjevski, Andrei; Inerbaev, Talgat; ...

2017-03-21

Methylammonium lead iodide perovskite (MAPbI 3) is a promising material for photovoltaic devices. A modification of MAPbI 3 into confined nanostructures is expected to further increase efficiency of solar energy conversion. Photoexcited dynamic processes in a MAPbI3 quantum dot (QD) have been modeled by many-body perturbation theory and nonadiabatic dynamics. A photoexcitation is followed by either exciton cooling (EC), its radiative (RR) or nonradiative recombination (NRR), or multiexciton generation (MEG) processes. Computed times of these processes fall in the order of MEG < EC < RR < NRR, where MEG is on the order of a few femtoseconds, EC ismore » in the picosecond range, while RR and NRR are on the order of nanoseconds. Computed time scales indicate which electronic transition pathways can contribute to increase in charge collection efficiency. Simulated mechanisms of relaxation and their rates show that quantum confinement promotes MEG in MAPbI 3 QDs.« less

Path-integral simulation of solids.

PubMed

Herrero, C P; Ramírez, R

2014-06-11

The path-integral formulation of the statistical mechanics of quantum many-body systems is described, with the purpose of introducing practical techniques for the simulation of solids. Monte Carlo and molecular dynamics methods for distinguishable quantum particles are presented, with particular attention to the isothermal-isobaric ensemble. Applications of these computational techniques to different types of solids are reviewed, including noble-gas solids (helium and heavier elements), group-IV materials (diamond and elemental semiconductors), and molecular solids (with emphasis on hydrogen and ice). Structural, vibrational, and thermodynamic properties of these materials are discussed. Applications also include point defects in solids (structure and diffusion), as well as nuclear quantum effects in solid surfaces and adsorbates. Different phenomena are discussed, as solid-to-solid and orientational phase transitions, rates of quantum processes, classical-to-quantum crossover, and various finite-temperature anharmonic effects (thermal expansion, isotopic effects, electron-phonon interactions). Nuclear quantum effects are most remarkable in the presence of light atoms, so that especial emphasis is laid on solids containing hydrogen as a constituent element or as an impurity.

Preferential sites for InAsP/InP quantum wire nucleation using molecular dynamics

NASA Astrophysics Data System (ADS)

Nuñez-Moraleda, Bernardo; Pizarro, Joaquin; Guerrero, Elisa; Guerrero-Lebrero, Maria P.; Yáñez, Andres; Molina, Sergio Ignacio; Galindo, Pedro Luis

2014-11-01

In this paper, stress fields at the surface of the capping layer of self-assembled InAsP quantum wires grown on an InP (001) substrate have been determined from atomistic models using molecular dynamics and Stillinger-Weber potentials. To carry out these calculations, the quantum wire compositional distribution was extracted from previous works, where the As and P distributions were determined by electron energy loss spectroscopy and high-resolution aberration-corrected Z-contrast imaging. Preferential sites for the nucleation of wires on the surface of the capping layer were studied and compared with (i) previous simulations using finite element analysis to solve anisotropic elastic theory equations and (ii) experimentally measured locations of stacked wires. Preferential nucleation sites of stacked wires were determined by the maximum stress location at the MD model surface in good agreement with experimental results and those derived from finite element analysis. This indicates that MD simulations based on empirical potentials provide a suitable and flexible tool to study strain dependent atom processes.

Quantum simulation of thermally-driven phase transition and oxygen K-edge x-ray absorption of high-pressure ice

PubMed Central

Kang, Dongdong; Dai, Jiayu; Sun, Huayang; Hou, Yong; Yuan, Jianmin

2013-01-01

The structure and phase transition of high-pressure ice are of long-standing interest and challenge, and there is still a huge gap between theoretical and experimental understanding. The quantum nature of protons such as delocalization, quantum tunneling and zero-point motion is crucial to the comprehension of the properties of high-pressure ice. Here we investigated the temperature-induced phase transition and oxygen K-edge x-ray absorption spectra of ice VII, VIII and X using ab initio path-integral molecular dynamics simulations. The tremendous difference between experiments and the previous theoretical predictions is closed for the phase diagram of ice below 300 K at pressures up to 110 GPa. Proton tunneling assists the proton-ordered ice VIII to transform into proton-disordered ice VII where only thermal activated proton-transfer cannot occur. The oxygen K edge with its shift is sensitive to the order-disorder transition, and therefore can be applied to diagnose the dynamics of ice structures. PMID:24253589

Bifurcation-based adiabatic quantum computation with a nonlinear oscillator network.

PubMed

Goto, Hayato

2016-02-22

The dynamics of nonlinear systems qualitatively change depending on their parameters, which is called bifurcation. A quantum-mechanical nonlinear oscillator can yield a quantum superposition of two oscillation states, known as a Schrödinger cat state, via quantum adiabatic evolution through its bifurcation point. Here we propose a quantum computer comprising such quantum nonlinear oscillators, instead of quantum bits, to solve hard combinatorial optimization problems. The nonlinear oscillator network finds optimal solutions via quantum adiabatic evolution, where nonlinear terms are increased slowly, in contrast to conventional adiabatic quantum computation or quantum annealing, where quantum fluctuation terms are decreased slowly. As a result of numerical simulations, it is concluded that quantum superposition and quantum fluctuation work effectively to find optimal solutions. It is also notable that the present computer is analogous to neural computers, which are also networks of nonlinear components. Thus, the present scheme will open new possibilities for quantum computation, nonlinear science, and artificial intelligence.

Bifurcation-based adiabatic quantum computation with a nonlinear oscillator network

NASA Astrophysics Data System (ADS)

Goto, Hayato

2016-02-01

The dynamics of nonlinear systems qualitatively change depending on their parameters, which is called bifurcation. A quantum-mechanical nonlinear oscillator can yield a quantum superposition of two oscillation states, known as a Schrödinger cat state, via quantum adiabatic evolution through its bifurcation point. Here we propose a quantum computer comprising such quantum nonlinear oscillators, instead of quantum bits, to solve hard combinatorial optimization problems. The nonlinear oscillator network finds optimal solutions via quantum adiabatic evolution, where nonlinear terms are increased slowly, in contrast to conventional adiabatic quantum computation or quantum annealing, where quantum fluctuation terms are decreased slowly. As a result of numerical simulations, it is concluded that quantum superposition and quantum fluctuation work effectively to find optimal solutions. It is also notable that the present computer is analogous to neural computers, which are also networks of nonlinear components. Thus, the present scheme will open new possibilities for quantum computation, nonlinear science, and artificial intelligence.

A molecular dynamics study of intramolecular proton transfer reaction of malonaldehyde in solutions based upon mixed quantum-classical approximation. I. Proton transfer reaction in water

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

Yamada, Atsushi; Kojima, Hidekazu; Okazaki, Susumu, E-mail: okazaki@apchem.nagoya-u.ac.jp

2014-08-28

In order to investigate proton transfer reaction in solution, mixed quantum-classical molecular dynamics calculations have been carried out based on our previously proposed quantum equation of motion for the reacting system [A. Yamada and S. Okazaki, J. Chem. Phys. 128, 044507 (2008)]. Surface hopping method was applied to describe forces acting on the solvent classical degrees of freedom. In a series of our studies, quantum and solvent effects on the reaction dynamics in solutions have been analysed in detail. Here, we report our mixed quantum-classical molecular dynamics calculations for intramolecular proton transfer of malonaldehyde in water. Thermally activated proton transfermore » process, i.e., vibrational excitation in the reactant state followed by transition to the product state and vibrational relaxation in the product state, as well as tunneling reaction can be described by solving the equation of motion. Zero point energy is, of course, included, too. The quantum simulation in water has been compared with the fully classical one and the wave packet calculation in vacuum. The calculated quantum reaction rate in water was 0.70 ps{sup −1}, which is about 2.5 times faster than that in vacuum, 0.27 ps{sup −1}. This indicates that the solvent water accelerates the reaction. Further, the quantum calculation resulted in the reaction rate about 2 times faster than the fully classical calculation, which indicates that quantum effect enhances the reaction rate, too. Contribution from three reaction mechanisms, i.e., tunneling, thermal activation, and barrier vanishing reactions, is 33:46:21 in the mixed quantum-classical calculations. This clearly shows that the tunneling effect is important in the reaction.« less

Reconfigurable optical implementation of quantum complex networks

NASA Astrophysics Data System (ADS)

Nokkala, J.; Arzani, F.; Galve, F.; Zambrini, R.; Maniscalco, S.; Piilo, J.; Treps, N.; Parigi, V.

2018-05-01

Network theory has played a dominant role in understanding the structure of complex systems and their dynamics. Recently, quantum complex networks, i.e. collections of quantum systems arranged in a non-regular topology, have been theoretically explored leading to significant progress in a multitude of diverse contexts including, e.g., quantum transport, open quantum systems, quantum communication, extreme violation of local realism, and quantum gravity theories. Despite important progress in several quantum platforms, the implementation of complex networks with arbitrary topology in quantum experiments is still a demanding task, especially if we require both a significant size of the network and the capability of generating arbitrary topology—from regular to any kind of non-trivial structure—in a single setup. Here we propose an all optical and reconfigurable implementation of quantum complex networks. The experimental proposal is based on optical frequency combs, parametric processes, pulse shaping and multimode measurements allowing the arbitrary control of the number of the nodes (optical modes) and topology of the links (interactions between the modes) within the network. Moreover, we also show how to simulate quantum dynamics within the network combined with the ability to address its individual nodes. To demonstrate the versatility of these features, we discuss the implementation of two recently proposed probing techniques for quantum complex networks and structured environments.

Quantum simulations of the Ising model with trapped ions: Devil's staircase and arbitrary lattice proposal

NASA Astrophysics Data System (ADS)

Korenblit, Simcha

A collection of trapped atomic ions represents one of the most attractive platforms for the quantum simulation of interacting spin networks and quantum magnetism. Spin-dependent optical dipole forces applied to an ion crystal create long-range effective spin-spin interactions and allow the simulation of spin Hamiltonians that possess nontrivial phases and dynamics. We trap linear chains of 171Yb+ ions in a Paul trap, and constrain the occupation of energy levels to the ground hyperne clock-states, creating a qubit or pseudo-spin 1/2 system. We proceed to implement spin-spin couplings between two ions using the far detuned Molmer-Sorenson scheme and perform adiabatic quantum simulations of Ising Hamiltonians with long-range couplings. We then demonstrate our ability to control the sign and relative strength of the interaction between three ions. Using this control, we simulate a frustrated triangular lattice, and for the first time establish an experimental connection between frustration and quantum entanglement. We then scale up our simulation to show phase transitions from paramagnetism to ferromagnetism for nine ions, and to anti-ferromagnetism for sixteen ions. The experimental work culminates with our most complicated Hamiltonian---a long range anti-ferromagnetic Ising interaction between 10 ions with a biasing axial field. Theoretical work presented in this thesis shows how the approach to quantum simulation utilized in this thesis can be further extended and improved. It is shown how appropriate design of laser fields can provide for arbitrary multidimensional spin-spin interaction graphs even for the case of a linear spatial array of ions. This scheme uses currently existing trap technology and is scalable to levels where classical methods of simulation are intractable.

Direct Quantum Mechanical Simulations of Shocked Energetic Materials

DTIC Science & Technology

2008-12-01

dynamics (QMD) simulations of shocked pentaerythritol tetranitrate (PETN), a conventional high explosive , and the polymeric cubic gauche phase of...nitrogen (cg-N), proposed as an environmentally acceptable energetic alternative to conventional explosive formulations. These simulations, made...stored structural potential energy can be liberated quickly enough, it is possible that explosion can occur with energies several orders of magnitude

Nonequilibrium dynamic critical scaling of the quantum Ising chain.

PubMed

Kolodrubetz, Michael; Clark, Bryan K; Huse, David A

2012-07-06

We solve for the time-dependent finite-size scaling functions of the one-dimensional transverse-field Ising chain during a linear-in-time ramp of the field through the quantum critical point. We then simulate Mott-insulating bosons in a tilted potential, an experimentally studied system in the same equilibrium universality class, and demonstrate that universality holds for the dynamics as well. We find qualitatively athermal features of the scaling functions, such as negative spin correlations, and we show that they should be robustly observable within present cold atom experiments.

Intermediate-band dynamics of quantum dots solar cell in concentrator photovoltaic modules

PubMed Central

Sogabe, Tomah; Shoji, Yasushi; Ohba, Mitsuyoshi; Yoshida, Katsuhisa; Tamaki, Ryo; Hong, Hwen-Fen; Wu, Chih-Hung; Kuo, Cherng-Tsong; Tomić, Stanko; Okada, Yoshitaka

2014-01-01

We report for the first time a successful fabrication and operation of an InAs/GaAs quantum dot based intermediate band solar cell concentrator photovoltaic (QD-IBSC-CPV) module to the IEC62108 standard with recorded power conversion efficiency of 15.3%. Combining the measured experimental results at Underwriters Laboratory (UL®) licensed testing laboratory with theoretical simulations, we confirmed that the operational characteristics of the QD-IBSC-CPV module are a consequence of the carrier dynamics via the intermediate-band at room temperature. PMID:24762433

Mixed quantum-classical simulation of the hydride transfer reaction catalyzed by dihydrofolate reductase based on a mapped system-harmonic bath model

NASA Astrophysics Data System (ADS)

Xu, Yang; Song, Kai; Shi, Qiang

2018-03-01

The hydride transfer reaction catalyzed by dihydrofolate reductase is studied using a recently developed mixed quantum-classical method to investigate the nuclear quantum effects on the reaction. Molecular dynamics simulation is first performed based on a two-state empirical valence bond potential to map the atomistic model to an effective double-well potential coupled to a harmonic bath. In the mixed quantum-classical simulation, the hydride degree of freedom is quantized, and the effective harmonic oscillator modes are treated classically. It is shown that the hydride transfer reaction rate using the mapped effective double-well/harmonic-bath model is dominated by the contribution from the ground vibrational state. Further comparison with the adiabatic reaction rate constant based on the Kramers theory confirms that the reaction is primarily vibrationally adiabatic, which agrees well with the high transmission coefficients found in previous theoretical studies. The calculated kinetic isotope effect is also consistent with the experimental and recent theoretical results.

Charge-state dynamics in electrostatic force spectroscopy

NASA Astrophysics Data System (ADS)

Ondráček, Martin; Hapala, Prokop; Jelínek, Pavel

2016-07-01

We present a numerical model that allows us to study the response of an oscillating probe in electrostatic force spectroscopy to charge switching in quantum dots at various time scales. The model provides more insight into the behavior of frequency shift and dissipated energy under different scanning conditions when measuring a temporarily charged quantum dot on a surface. Namely, we analyze the dependence of the frequency shift, the dissipated energy, and their fluctuations on the resonance frequency of the tip and on the electron tunneling rates across the tip-quantum dot and quantum dot-sample junctions. We discuss two complementary approaches to simulating the charge dynamics, a stochastic and a deterministic one. In addition, we derive analytic formulas valid for small amplitudes, describing relations between the frequency shift, dissipated energy, and the characteristic rates driving the charging and discharging processes.

Role of Quantum Vibrations on the Structural, Electronic, and Optical Properties of 9-Methylguanine.

PubMed

Law, Yu Kay; Hassanali, Ali A

2015-11-05

In this work, we report theoretical predictions of the UV-absorption spectra of 9-methylguanine using time dependent density functional theory (TDDFT). Molecular dynamics simulations of the hydrated DNA base are peformed using an empirical force field, Born-Oppenheimer ab initio molecular dynamics (AIMD), and finally path-integral AIMD to understand the role of the underlying electronic potential, solvation, and nuclear quantum vibrations on the absorption spectra. It is shown that the conformational distributions, including hydrogen bonding interactions, are perturbed by the inclusion of nuclear quantum effects, leading to significant changes in the total charge and dipole fluctuations of the DNA base. The calculated absorption spectra using the different sampling protocols shows that the inclusion of nuclear quantum effects causes a significant broadening and red shift of the spectra bringing it into closer agreement with experiments.

Out-of-equilibrium dynamics driven by localized time-dependent perturbations at quantum phase transitions

NASA Astrophysics Data System (ADS)

Pelissetto, Andrea; Rossini, Davide; Vicari, Ettore

2018-03-01

We investigate the quantum dynamics of many-body systems subject to local (i.e., restricted to a limited space region) time-dependent perturbations. If the system crosses a quantum phase transition, an off-equilibrium behavior is observed, even for a very slow driving. We show that, close to the transition, time-dependent quantities obey scaling laws. In first-order transitions, the scaling behavior is universal, and some scaling functions can be computed exactly. For continuous transitions, the scaling laws are controlled by the standard critical exponents and by the renormalization-group dimension of the perturbation at the transition. Our protocol can be implemented in existing relatively small quantum simulators, paving the way for a quantitative probe of the universal off-equilibrium scaling behavior, without the need to manipulate systems close to the thermodynamic limit.

Polarizable Force Field for DNA Based on the Classical Drude Oscillator: I. Refinement Using Quantum Mechanical Base Stacking and Conformational Energetics.

PubMed

Lemkul, Justin A; MacKerell, Alexander D

2017-05-09

Empirical force fields seek to relate the configuration of a set of atoms to its energy, thus yielding the forces governing its dynamics, using classical physics rather than more expensive quantum mechanical calculations that are computationally intractable for large systems. Most force fields used to simulate biomolecular systems use fixed atomic partial charges, neglecting the influence of electronic polarization, instead making use of a mean-field approximation that may not be transferable across environments. Recent hardware and software developments make polarizable simulations feasible, and to this end, polarizable force fields represent the next generation of molecular dynamics simulation technology. In this work, we describe the refinement of a polarizable force field for DNA based on the classical Drude oscillator model by targeting quantum mechanical interaction energies and conformational energy profiles of model compounds necessary to build a complete DNA force field. The parametrization strategy employed in the present work seeks to correct weak base stacking in A- and B-DNA and the unwinding of Z-DNA observed in the previous version of the force field, called Drude-2013. Refinement of base nonbonded terms and reparametrization of dihedral terms in the glycosidic linkage, deoxyribofuranose rings, and important backbone torsions resulted in improved agreement with quantum mechanical potential energy surfaces. Notably, we expand on previous efforts by explicitly including Z-DNA conformational energetics in the refinement.

Atomic-scale investigation of nuclear quantum effects of surface water: Experiments and theory

NASA Astrophysics Data System (ADS)

Guo, Jing; Li, Xin-Zheng; Peng, Jinbo; Wang, En-Ge; Jiang, Ying

2017-12-01

Quantum behaviors of protons in terms of tunneling and zero-point motion have significant effects on the macroscopic properties, structure, and dynamics of water even at room temperature or higher. In spite of tremendous theoretical and experimental efforts, accurate and quantitative description of the nuclear quantum effects (NQEs) is still challenging. The main difficulty lies in that the NQEs are extremely susceptible to the structural inhomogeneity and local environments, especially when interfacial systems are concerned. In this review article, we will highlight the recent advances of scanning tunneling microscopy and spectroscopy (STM/S), which allows the access to the quantum degree of freedom of protons both in real and energy space. In addition, we will also introduce recent development of ab initio path-integral molecular dynamics (PIMD) simulations at surfaces/interfaces, in which both the electrons and nuclei are treated as quantum particles in contrast to traditional ab initio molecular dynamics (MD). Then we will discuss how the combination of STM/S and PIMD are used to directly visualize the concerted quantum tunneling of protons within the water clusters and quantify the impact of zero-point motion on the strength of a single hydrogen bond (H bond) at a water/solid interface. Those results may open up the new possibility of exploring the exotic quantum states of light nuclei at surfaces, as well as the quantum coupling between the electrons and nuclei.

A theory of quantum dynamics of a nanomagnet under excitation

NASA Astrophysics Data System (ADS)

Sham, L. J.

2013-09-01

A quantum treatment of magnetization dynamics of a nanomagnet between a thousand and a million spins may be needed as the magnet interacts with quantum control. The advantage of the all-quantum approach over the classical treatment of magnetization is the accounting for the correlation between the magnet and the control agent and the first-principles source of noise. This supplement to the conference talk will concentrate on an overview of the theory with a presentation of the basic ideas which could have wide applications and illustrations with some results. Details of applications to specific models are or will be published elsewhere. A clear concept of the structure of the ground and excited macrospin states as magnetization rotation states and magnons in the Bloch/Dyson sense gives rise to a consistent theory of the magnetization dynamics of a ferromagnet modeled by the Heisenberg Hamiltonian. An example of quantum control is the spin torque transfer, treated here as a sequence of scatterings of each current electron with the localized electrons of the ferromagnet, yields in each encounter a probability distribution of the magnetization recoil state correlated with each outgoing state of the electron. This picture provides a natural Monte Carlo process for simulation of the dynamics in which the probability is determined by quantum mechanics. The computed results of mean motion, noise and damping of the magnetization will be discussed.

Theoretical approaches for dynamical ordering of biomolecular systems.

PubMed

Okumura, Hisashi; Higashi, Masahiro; Yoshida, Yuichiro; Sato, Hirofumi; Akiyama, Ryo

2018-02-01

Living systems are characterized by the dynamic assembly and disassembly of biomolecules. The dynamical ordering mechanism of these biomolecules has been investigated both experimentally and theoretically. The main theoretical approaches include quantum mechanical (QM) calculation, all-atom (AA) modeling, and coarse-grained (CG) modeling. The selected approach depends on the size of the target system (which differs among electrons, atoms, molecules, and molecular assemblies). These hierarchal approaches can be combined with molecular dynamics (MD) simulation and/or integral equation theories for liquids, which cover all size hierarchies. We review the framework of quantum mechanical/molecular mechanical (QM/MM) calculations, AA MD simulations, CG modeling, and integral equation theories. Applications of these methods to the dynamical ordering of biomolecular systems are also exemplified. The QM/MM calculation enables the study of chemical reactions. The AA MD simulation, which omits the QM calculation, can follow longer time-scale phenomena. By reducing the number of degrees of freedom and the computational cost, CG modeling can follow much longer time-scale phenomena than AA modeling. Integral equation theories for liquids elucidate the liquid structure, for example, whether the liquid follows a radial distribution function. These theoretical approaches can analyze the dynamic behaviors of biomolecular systems. They also provide useful tools for exploring the dynamic ordering systems of biomolecules, such as self-assembly. This article is part of a Special Issue entitled "Biophysical Exploration of Dynamical Ordering of Biomolecular Systems" edited by Dr. Koichi Kato. Copyright © 2017 Elsevier B.V. All rights reserved.

Control aspects of quantum computing using pure and mixed states.

PubMed

Schulte-Herbrüggen, Thomas; Marx, Raimund; Fahmy, Amr; Kauffman, Louis; Lomonaco, Samuel; Khaneja, Navin; Glaser, Steffen J

2012-10-13

Steering quantum dynamics such that the target states solve classically hard problems is paramount to quantum simulation and computation. And beyond, quantum control is also essential to pave the way to quantum technologies. Here, important control techniques are reviewed and presented in a unified frame covering quantum computational gate synthesis and spectroscopic state transfer alike. We emphasize that it does not matter whether the quantum states of interest are pure or not. While pure states underly the design of quantum circuits, ensemble mixtures of quantum states can be exploited in a more recent class of algorithms: it is illustrated by characterizing the Jones polynomial in order to distinguish between different (classes of) knots. Further applications include Josephson elements, cavity grids, ion traps and nitrogen vacancy centres in scenarios of closed as well as open quantum systems.

Control aspects of quantum computing using pure and mixed states

PubMed Central

Schulte-Herbrüggen, Thomas; Marx, Raimund; Fahmy, Amr; Kauffman, Louis; Lomonaco, Samuel; Khaneja, Navin; Glaser, Steffen J.

2012-01-01

Steering quantum dynamics such that the target states solve classically hard problems is paramount to quantum simulation and computation. And beyond, quantum control is also essential to pave the way to quantum technologies. Here, important control techniques are reviewed and presented in a unified frame covering quantum computational gate synthesis and spectroscopic state transfer alike. We emphasize that it does not matter whether the quantum states of interest are pure or not. While pure states underly the design of quantum circuits, ensemble mixtures of quantum states can be exploited in a more recent class of algorithms: it is illustrated by characterizing the Jones polynomial in order to distinguish between different (classes of) knots. Further applications include Josephson elements, cavity grids, ion traps and nitrogen vacancy centres in scenarios of closed as well as open quantum systems. PMID:22946034

Using quantum dynamics simulations to follow the competition between charge migration and charge transfer in polyatomic molecules

NASA Astrophysics Data System (ADS)

Spinlove, K. E.; Vacher, M.; Bearpark, M.; Robb, M. A.; Worth, G. A.

2017-01-01

Recent work, particularly by Cederbaum and co-workers, has identified the phenomenon of charge migration, whereby charge flow occurs over a static molecular framework after the creation of an electronic wavepacket. In a real molecule, this charge migration competes with charge transfer, whereby the nuclear motion also results in the re-distribution of charge. To study this competition, quantum dynamics simulations need to be performed. To break the exponential scaling of standard grid-based algorithms, approximate methods need to be developed that are efficient yet able to follow the coupled electronic-nuclear motion of these systems. Using a simple model Hamiltonian based on the ionisation of the allene molecule, the performance of different methods based on Gaussian Wavepackets is demonstrated.

Quantum mechanical/molecular mechanical molecular dynamics and free energy simulations of the thiopurine S-methyltransferase reaction with 6-mercaptopurine.

PubMed

Pan, Xiao-Liang; Cui, Feng-Chao; Liu, Jing-Yao

2011-06-23

Quantum mechanical/molecular mechanical (QM/MM) molecular dynamics simulations were performed to investigate the methylation of 6-mercaptopurine catalyzed by thiopurine S-methyltransferase. Several setups with different tautomeric forms and orientations of the substrate were considered. It is found that, with the orientation in chain A of the X-ray structure, the substrate can form an ideal near-attack configuration for the methylation reaction, which may take place after the deprotonation of the substrate by the conserved residue Asp23 through a water chain. The potential of mean force (PMF) of the methyl-transfer step for the most favorable pathway is 19.6 kcal/mol, which is in good agreement with the available experimental rate constant data.

Effect of carbon spacer length on zwitterionic carboxybetaines.

PubMed

Shao, Qing; Jiang, Shaoyi

2013-02-07

Zwitterionic carboxybetaines (CBs) are ubiquitous in nature and considered promising materials for biological and chemical applications. A thorough understanding of the effect of carbon spacer length (CSL) on molecular properties is important. In this work, using molecular dynamics simulation and quantum chemical calculation, we investigated the effect of CSL on the molecular properties of CB molecules. The hydration number, structure, and dynamics of carboxylic and trimethyl ammonium groups were investigated and found to present different behaviors in regards to the variation of CSL. The simulation results with partial charges developed from quantum chemical calculations were compared with those with partial charges from the OPLS all atom (OPLSAA) force field. The hydration free energy of CB molecules and CB-Na(+) association was also studied as a function of CSL.

A quantum relativistic battle of the sexes cellular automaton

NASA Astrophysics Data System (ADS)

Alonso-Sanz, Ramón; Situ, Haozhen

2017-02-01

The effect of variable entangling on the dynamics of a spatial quantum relativistic formulation of the iterated battle of the sexes game is studied in this work. The game is played in the cellular automata manner, i.e., with local and synchronous interaction. The game is assessed in fair and unfair contests. Despite the full range of quantum parameters initially accessible, they promptly converge into fairly stable configurations, that often show rich spatial structures in simulations with no negligible entanglement.

The importance of nuclear quantum effects in spectral line broadening of optical spectra and electrostatic properties in aromatic chromophores.

PubMed

Law, Y K; Hassanali, A A

2018-03-14

In this work, we examine the importance of nuclear quantum effects on capturing the line broadening and vibronic structure of optical spectra. We determine the absorption spectra of three aromatic molecules indole, pyridine, and benzene using time dependent density functional theory with several molecular dynamics sampling protocols: force-field based empirical potentials, ab initio simulations, and finally path-integrals for the inclusion of nuclear quantum effects. We show that the absorption spectrum for all these chromophores are similarly broadened in the presence of nuclear quantum effects regardless of the presence of hydrogen bond donor or acceptor groups. We also show that simulations incorporating nuclear quantum effects are able to reproduce the heterogeneous broadening of the absorption spectra even with empirical force fields. The spectral broadening associated with nuclear quantum effects can be accounted for by the broadened distribution of chromophore size as revealed by a particle in the box model. We also highlight the role that nuclear quantum effects have on the underlying electronic structure of aromatic molecules as probed by various electrostatic properties.

The importance of nuclear quantum effects in spectral line broadening of optical spectra and electrostatic properties in aromatic chromophores

NASA Astrophysics Data System (ADS)

Law, Y. K.; Hassanali, A. A.

2018-03-01

In this work, we examine the importance of nuclear quantum effects on capturing the line broadening and vibronic structure of optical spectra. We determine the absorption spectra of three aromatic molecules indole, pyridine, and benzene using time dependent density functional theory with several molecular dynamics sampling protocols: force-field based empirical potentials, ab initio simulations, and finally path-integrals for the inclusion of nuclear quantum effects. We show that the absorption spectrum for all these chromophores are similarly broadened in the presence of nuclear quantum effects regardless of the presence of hydrogen bond donor or acceptor groups. We also show that simulations incorporating nuclear quantum effects are able to reproduce the heterogeneous broadening of the absorption spectra even with empirical force fields. The spectral broadening associated with nuclear quantum effects can be accounted for by the broadened distribution of chromophore size as revealed by a particle in the box model. We also highlight the role that nuclear quantum effects have on the underlying electronic structure of aromatic molecules as probed by various electrostatic properties.

First-Principle Simulations of Water

NASA Astrophysics Data System (ADS)

Schwegler, Eric

2004-03-01

The structural and dynamical properties of water are investigated with a series of first-principle and classical molecular dynamics simulations. A number of effects that can influence the simulated properties of water will be discussed including temperature, intramolecular flexibility [1], and the quantum nature of protons. This work was performed under the auspices of the U.S. Dept. of Energy at the University of California/Lawrence Livermore National Laboratory under contract no. W-7405-Eng-48. [1] M. Allesch, E. Schwegler, G. Galli, F. Gygi, J. Chem. Phys. in press 2004.

Light-induced nonadiabatic dynamics in molecular assemblies and nanostructures

NASA Astrophysics Data System (ADS)

Mitric, Roland

The combination of mixed quantum-classical dynamics with efficient electronic structure methods was developed in order to simulate the light-induced processes in complex molecules, multichromophoric aggregates and metallic nanostructures. We will demonstrate how the combination of nonadiabatic dynamics with experimental pump-probe techniques such as time-resolved photoelectron imaging (TRPEI) allows to fully resolve the mechanism of excited state relaxation through conical intersections in several prototype organic- and biomolecules. Specifically, the role of the solvent in the excited state relaxation in microsolvated and fully solvated systems will be addressed. Currently there is growing evidence that nonadiabatic relaxation processes also play a fundamental role in determining the efficiency of excitonic transfer or charge injection in multichromophoric assemblies. Since such systems are currently out of the reach of the state-of-the-art quantum chemistry a development of even more efficient quantum chemical approaches is necessary in order to describe the excited state dynamics in such assemblies. For this purpose we have recently developed long-range corrected time-dependent density functional tight binding (LC-TDDFTB) nonadiabatic dynamics and combined it with the QM/MM approach in order to simulate exciton relaxation in complex systems. The applications of the method to the investigation of the optical properties and dynamics in multichromophoric assemblies including stacked pi-conjugated organic chromophores, model molecular crystals as well as self-organized dye aggregates will be presented. Finally, we will address exciton transport dynamics coupled with the light propagation in hybrid exciton-plasmon nanostructures, which represent promising materials fort the development of novel light-harvesting systems.

Control of Electronic Structures and Phonon Dynamics in Quantum Dot Superlattices by Manipulation of Interior Nanospace.

PubMed

Chang, I-Ya; Kim, DaeGwi; Hyeon-Deuk, Kim

2016-07-20

Quantum dot (QD) superlattices, periodically ordered array structures of QDs, are expected to provide novel photo-optical functions due to their resonant couplings between adjacent QDs. Here, we computationally demonstrated that electronic structures and phonon dynamics of a QD superlattice can be effectively and selectively controlled by manipulating its interior nanospace, where quantum resonance between neighboring QDs appears, rather than by changing component QD size, shape, compositions, etc. A simple H-passivated Si QD was examined to constitute one-, two-, and three-dimensional QD superlattices, and thermally fluctuating band energies and phonon modes were simulated by finite-temperature ab initio molecular dynamics (MD) simulations. The QD superlattice exhibited a decrease in the band gap energy enhanced by thermal modulations and also exhibited selective extraction of charge carriers out of the component QD, indicating its advantage as a promising platform for implementation in solar cells. Our dynamical phonon analyses based on the ab initio MD simulations revealed that THz-frequency phonon modes were created by an inter-QD crystalline lattice formed in the QD superlattice, which can contribute to low energy thermoelectric conversion and will be useful for direct observation of the dimension-dependent superlattice. Further, we found that crystalline and ligand-originated phonon modes inside each component QD can be independently controlled by asymmetry of the superlattice and by restriction of the interior nanospace, respectively. Taking into account the thermal effects at the finite temperature, we proposed guiding principles for designing efficient and space-saving QD superlattices to develop functional photovoltaic and thermoelectric devices.

Variational mixed quantum/semiclassical simulation of dihalogen guest and rare-gas solid host dynamics

NASA Astrophysics Data System (ADS)

Cheng, Xiaolu; Cina, Jeffrey A.

2014-07-01

A variational mixed quantum-semiclassical theory for the internal nuclear dynamics of a small molecule and the induced small-amplitude coherent motion of a low-temperature host medium is developed, tested, and used to simulate the temporal evolution of nonstationary states of the internal molecular and surrounding medium degrees of freedom. In this theory, termed the Fixed Vibrational Basis/Gaussian Bath (FVB/GB) method, the system is treated fully quantum mechanically while Gaussian wave packets are used for the bath degrees of freedom. An approximate time-dependent wave function of the entire model is obtained instead of just a reduced system density matrix, so the theory enables the analysis of the entangled system and bath dynamics that ensues following initial displacement of the internal-molecular (system) coordinate from its equilibrium position. The norm- and energy-conserving properties of the propagation of our trial wave function are natural consequences of the Dirac-Frenkel-McLachlan variational principle. The variational approach also stabilizes the time evolution in comparison to the same ansatz propagated under a previously employed locally quadratic approximation to the bath potential and system-bath interaction terms in the bath-parameter equations of motion. Dynamics calculations are carried out for molecular iodine in a 2D krypton lattice that reveal both the time-course of vibrational decoherence and the details of host-atom motion accompanying energy dissipation and dephasing. This work sets the stage for the comprehensive simulation of ultrafast time-resolved optical experiments on small molecules in low-temperature solids.

Molecular Dynamics Simulations with Quantum Mechanics/Molecular Mechanics and Adaptive Neural Networks.

PubMed

Shen, Lin; Yang, Weitao

2018-03-13

Direct molecular dynamics (MD) simulation with ab initio quantum mechanical and molecular mechanical (QM/MM) methods is very powerful for studying the mechanism of chemical reactions in a complex environment but also very time-consuming. The computational cost of QM/MM calculations during MD simulations can be reduced significantly using semiempirical QM/MM methods with lower accuracy. To achieve higher accuracy at the ab initio QM/MM level, a correction on the existing semiempirical QM/MM model is an attractive idea. Recently, we reported a neural network (NN) method as QM/MM-NN to predict the potential energy difference between semiempirical and ab initio QM/MM approaches. The high-level results can be obtained using neural network based on semiempirical QM/MM MD simulations, but the lack of direct MD samplings at the ab initio QM/MM level is still a deficiency that limits the applications of QM/MM-NN. In the present paper, we developed a dynamic scheme of QM/MM-NN for direct MD simulations on the NN-predicted potential energy surface to approximate ab initio QM/MM MD. Since some configurations excluded from the database for NN training were encountered during simulations, which may cause some difficulties on MD samplings, an adaptive procedure inspired by the selection scheme reported by Behler [ Behler Int. J. Quantum Chem. 2015 , 115 , 1032 ; Behler Angew. Chem., Int. Ed. 2017 , 56 , 12828 ] was employed with some adaptions to update NN and carry out MD iteratively. We further applied the adaptive QM/MM-NN MD method to the free energy calculation and transition path optimization on chemical reactions in water. The results at the ab initio QM/MM level can be well reproduced using this method after 2-4 iteration cycles. The saving in computational cost is about 2 orders of magnitude. It demonstrates that the QM/MM-NN with direct MD simulations has great potentials not only for the calculation of thermodynamic properties but also for the characterization of reaction dynamics, which provides a useful tool to study chemical or biochemical systems in solution or enzymes.

Practical recipes for the model order reduction, dynamical simulation and compressive sampling of large-scale open quantum systems

NASA Astrophysics Data System (ADS)

Sidles, John A.; Garbini, Joseph L.; Harrell, Lee E.; Hero, Alfred O.; Jacky, Jonathan P.; Malcomb, Joseph R.; Norman, Anthony G.; Williamson, Austin M.

2009-06-01

Practical recipes are presented for simulating high-temperature and nonequilibrium quantum spin systems that are continuously measured and controlled. The notion of a spin system is broadly conceived, in order to encompass macroscopic test masses as the limiting case of large-j spins. The simulation technique has three stages: first the deliberate introduction of noise into the simulation, then the conversion of that noise into an equivalent continuous measurement and control process, and finally, projection of the trajectory onto state-space manifolds having reduced dimensionality and possessing a Kähler potential of multilinear algebraic form. These state-spaces can be regarded as ruled algebraic varieties upon which a projective quantum model order reduction (MOR) is performed. The Riemannian sectional curvature of ruled Kählerian varieties is analyzed, and proved to be non-positive upon all sections that contain a rule. These manifolds are shown to contain Slater determinants as a special case and their identity with Grassmannian varieties is demonstrated. The resulting simulation formalism is used to construct a positive P-representation for the thermal density matrix. Single-spin detection by magnetic resonance force microscopy (MRFM) is simulated, and the data statistics are shown to be those of a random telegraph signal with additive white noise. Larger-scale spin-dust models are simulated, having no spatial symmetry and no spatial ordering; the high-fidelity projection of numerically computed quantum trajectories onto low dimensionality Kähler state-space manifolds is demonstrated. The reconstruction of quantum trajectories from sparse random projections is demonstrated, the onset of Donoho-Stodden breakdown at the Candès-Tao sparsity limit is observed, a deterministic construction for sampling matrices is given and methods for quantum state optimization by Dantzig selection are given.

High performance computing in biology: multimillion atom simulations of nanoscale systems

PubMed Central

Sanbonmatsu, K. Y.; Tung, C.-S.

2007-01-01

Computational methods have been used in biology for sequence analysis (bioinformatics), all-atom simulation (molecular dynamics and quantum calculations), and more recently for modeling biological networks (systems biology). Of these three techniques, all-atom simulation is currently the most computationally demanding, in terms of compute load, communication speed, and memory load. Breakthroughs in electrostatic force calculation and dynamic load balancing have enabled molecular dynamics simulations of large biomolecular complexes. Here, we report simulation results for the ribosome, using approximately 2.64 million atoms, the largest all-atom biomolecular simulation published to date. Several other nanoscale systems with different numbers of atoms were studied to measure the performance of the NAMD molecular dynamics simulation program on the Los Alamos National Laboratory Q Machine. We demonstrate that multimillion atom systems represent a 'sweet spot' for the NAMD code on large supercomputers. NAMD displays an unprecedented 85% parallel scaling efficiency for the ribosome system on 1024 CPUs. We also review recent targeted molecular dynamics simulations of the ribosome that prove useful for studying conformational changes of this large biomolecular complex in atomic detail. PMID:17187988

Nuclear quantum effects in water exchange around lithium and fluoride ions

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

Wilkins, David M.; Manolopoulos, David; Dang, Liem X.

2015-02-14

We employ classical and ring polymer molecular dynamics simulations to study the effect of nuclear quantum fluctuations on the structure and the water exchange dynamics of aqueous solutions of lithium and fluoride ions. While we obtain reasonably good agreement with experimental data for solutions of lithium by augmenting the Coulombic interactions between the ion and the water molecules with a standard Lennard-Jones ion-oxygen potential, the same is not true for solutions of fluoride, for which we find that a potential with a softer repulsive wall gives much better agreement. A small degree of destabilization of the first hydration shell ismore » found in quantum simulations of both ions when compared with classical simulations, with the shell becoming less sharply defined and the mean residence time of the water molecules in the shell decreasing. In line with these modest differences, we find that the mechanisms of the water exchange reactions are unaffected by quantization, so a classical description of these reactions gives qualitatively correct and quantitatively reasonable results. We also find that the quantum effects in solutions of lithium are larger than in solutions of fluoride. This is partly due to the stronger interaction of lithium with water molecules, partly due to the lighter mass of lithium, and partly due to competing quantum effects in the hydration of fluoride, which are absent in the hydration of lithium. LXD was supported by US Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences.« less

U(1) Wilson lattice gauge theories in digital quantum simulators

NASA Astrophysics Data System (ADS)

Muschik, Christine; Heyl, Markus; Martinez, Esteban; Monz, Thomas; Schindler, Philipp; Vogell, Berit; Dalmonte, Marcello; Hauke, Philipp; Blatt, Rainer; Zoller, Peter

2017-10-01

Lattice gauge theories describe fundamental phenomena in nature, but calculating their real-time dynamics on classical computers is notoriously difficult. In a recent publication (Martinez et al 2016 Nature 534 516), we proposed and experimentally demonstrated a digital quantum simulation of the paradigmatic Schwinger model, a U(1)-Wilson lattice gauge theory describing the interplay between fermionic matter and gauge bosons. Here, we provide a detailed theoretical analysis of the performance and the potential of this protocol. Our strategy is based on analytically integrating out the gauge bosons, which preserves exact gauge invariance but results in complicated long-range interactions between the matter fields. Trapped-ion platforms are naturally suited to implementing these interactions, allowing for an efficient quantum simulation of the model, with a number of gate operations that scales polynomially with system size. Employing numerical simulations, we illustrate that relevant phenomena can be observed in larger experimental systems, using as an example the production of particle-antiparticle pairs after a quantum quench. We investigate theoretically the robustness of the scheme towards generic error sources, and show that near-future experiments can reach regimes where finite-size effects are insignificant. We also discuss the challenges in quantum simulating the continuum limit of the theory. Using our scheme, fundamental phenomena of lattice gauge theories can be probed using a broad set of experimentally accessible observables, including the entanglement entropy and the vacuum persistence amplitude.

Digital-analog quantum simulation of generalized Dicke models with superconducting circuits

NASA Astrophysics Data System (ADS)

Lamata, Lucas

We propose a digital-analog quantum simulation of generalized Dicke models with superconducting circuits, including Fermi-Bose condensates, biased and pulsed Dicke models, for all regimes of light-matter coupling. We encode these classes of problems in a set of superconducting qubits coupled with a bosonic mode implemented by a transmission line resonator. Via digital-analog techniques, an efficient quantum simulation can be performed in state-of-the-art circuit quantum electrodynamics platforms, by suitable decomposition into analog qubit-bosonic blocks and collective single-qubit pulses through digital steps. Moreover, just a single global analog block would be needed during the whole protocol in most of the cases, superimposed with fast periodic pulses to rotate and detune the qubits. Therefore, a large number of digital steps may be attained with this approach, providing a reduced digital error. Additionally, the number of gates per digital step does not grow with the number of qubits, rendering the simulation efficient. This strategy paves the way for the scalable digital-analog quantum simulation of many-body dynamics involving bosonic modes and spin degrees of freedom with superconducting circuits. The author wishes to acknowledge discussions with I. Arrazola, A. Mezzacapo, J. S. Pedernales, and E. Solano, and support from Ramon y Cajal Grant RYC-2012-11391, Spanish MINECO/FEDER FIS2015-69983-P, UPV/EHU UFI 11/55 and Project EHUA14/04.

Fragmentation-based QM/MM simulations: length dependence of chain dynamics and hydrogen bonding of polyethylene oxide and polyethylene in aqueous solutions.

PubMed

Li, Hui; Li, Wei; Li, Shuhua; Ma, Jing

2008-06-12

Molecular fragmentation quantum mechanics (QM) calculations have been combined with molecular mechanics (MM) to construct the fragmentation QM/MM method for simulations of dilute solutions of macromolecules. We adopt the electrostatics embedding QM/MM model, where the low-cost generalized energy-based fragmentation calculations are employed for the QM part. Conformation energy calculations, geometry optimizations, and Born-Oppenheimer molecular dynamics simulations of poly(ethylene oxide), PEO(n) (n = 6-20), and polyethylene, PE(n) ( n = 9-30), in aqueous solution have been performed within the framework of both fragmentation and conventional QM/MM methods. The intermolecular hydrogen bonding and chain configurations obtained from the fragmentation QM/MM simulations are consistent with the conventional QM/MM method. The length dependence of chain conformations and dynamics of PEO and PE oligomers in aqueous solutions is also investigated through the fragmentation QM/MM molecular dynamics simulations.

Dynamical gauge effects in an open quantum network

NASA Astrophysics Data System (ADS)

Zhao, Jianshi; Price, Craig; Liu, Qi; Gemelke, Nathan

2016-05-01

We describe new experimental techniques for simulation of high-energy field theories based on an analogy between open thermodynamic systems and effective dynamical gauge-fields following SU(2) × U(1) Yang-Mills models. By coupling near-resonant laser-modes to atoms moving in a disordered optical environment, we create an open system which exhibits a non-equilibrium phase transition between two steady-state behaviors, exhibiting scale-invariant behavior near the transition. By measuring transport of atoms through the disordered network, we observe two distinct scaling behaviors, corresponding to the classical and quantum limits for the dynamical gauge field. This behavior is loosely analogous to dynamical gauge effects in quantum chromodynamics, and can mapped onto generalized open problems in theoretical understanding of quantized non-Abelian gauge theories. Additional, the scaling behavior can be understood from the geometric structure of the gauge potential and linked to the measure of information in the local disordered potential, reflecting an underlying holographic principle. We acknowledge support from NSF Award No.1068570, and the Charles E. Kaufman Foundation.

Projective simulation for artificial intelligence

NASA Astrophysics Data System (ADS)

Briegel, Hans J.; de Las Cuevas, Gemma

2012-05-01

We propose a model of a learning agent whose interaction with the environment is governed by a simulation-based projection, which allows the agent to project itself into future situations before it takes real action. Projective simulation is based on a random walk through a network of clips, which are elementary patches of episodic memory. The network of clips changes dynamically, both due to new perceptual input and due to certain compositional principles of the simulation process. During simulation, the clips are screened for specific features which trigger factual action of the agent. The scheme is different from other, computational, notions of simulation, and it provides a new element in an embodied cognitive science approach to intelligent action and learning. Our model provides a natural route for generalization to quantum-mechanical operation and connects the fields of reinforcement learning and quantum computation.

Projective simulation for artificial intelligence

PubMed Central

Briegel, Hans J.; De las Cuevas, Gemma

2012-01-01

We propose a model of a learning agent whose interaction with the environment is governed by a simulation-based projection, which allows the agent to project itself into future situations before it takes real action. Projective simulation is based on a random walk through a network of clips, which are elementary patches of episodic memory. The network of clips changes dynamically, both due to new perceptual input and due to certain compositional principles of the simulation process. During simulation, the clips are screened for specific features which trigger factual action of the agent. The scheme is different from other, computational, notions of simulation, and it provides a new element in an embodied cognitive science approach to intelligent action and learning. Our model provides a natural route for generalization to quantum-mechanical operation and connects the fields of reinforcement learning and quantum computation. PMID:22590690

Real-time dynamics of matrix quantum mechanics beyond the classical approximation

NASA Astrophysics Data System (ADS)

Buividovich, Pavel; Hanada, Masanori; Schäfer, Andreas

2018-03-01

We describe a numerical method which allows to go beyond the classical approximation for the real-time dynamics of many-body systems by approximating the many-body Wigner function by the most general Gaussian function with time-dependent mean and dispersion. On a simple example of a classically chaotic system with two degrees of freedom we demonstrate that this Gaussian state approximation is accurate for significantly smaller field strengths and longer times than the classical one. Applying this approximation to matrix quantum mechanics, we demonstrate that the quantum Lyapunov exponents are in general smaller than their classical counterparts, and even seem to vanish below some temperature. This behavior resembles the finite-temperature phase transition which was found for this system in Monte-Carlo simulations, and ensures that the system does not violate the Maldacena-Shenker-Stanford bound λL < 2πT, which inevitably happens for classical dynamics at sufficiently small temperatures.

On the role of quantum ion dynamics for the anomalous melting of lithium

NASA Astrophysics Data System (ADS)

Elatresh, Sabri; Bonev, Stanimir

2011-03-01

Lithium has attracted a lot of interest in relation to a number of counterintuitive electronic and structural changes that it exhibits under pressure. One of the most remarkable properties of dense lithium is its anomalous melting. This behavior was first predicted theoretically based on first-principles molecular dynamics (FPMD) simulations, which treated the ions classically. The lowest melting temperature was determined to be about 275~K at 65~GPa. Recent experiments measured a melting temperature about 100~K lower at the same pressure. In this talk, we will present FPMD calculations of solid and liquid lithium free energies up to 100 GPa that take into account ion quantum dynamics. We examine the significance of the quantum effects for the finite-temperature phase boundaries of lithium and, in particular, its melting curve. Work supported by NSERC, Acenet, and LLNL under Contract DE-AC52-07NA27344.

Quantum-Inspired Maximizer

NASA Technical Reports Server (NTRS)

Zak, Michail

2008-01-01

A report discusses an algorithm for a new kind of dynamics based on a quantum- classical hybrid-quantum-inspired maximizer. The model is represented by a modified Madelung equation in which the quantum potential is replaced by different, specially chosen 'computational' potential. As a result, the dynamics attains both quantum and classical properties: it preserves superposition and entanglement of random solutions, while allowing one to measure its state variables, using classical methods. Such optimal combination of characteristics is a perfect match for quantum-inspired computing. As an application, an algorithm for global maximum of an arbitrary integrable function is proposed. The idea of the proposed algorithm is very simple: based upon the Quantum-inspired Maximizer (QIM), introduce a positive function to be maximized as the probability density to which the solution is attracted. Then the larger value of this function will have the higher probability to appear. Special attention is paid to simulation of integer programming and NP-complete problems. It is demonstrated that the problem of global maximum of an integrable function can be found in polynomial time by using the proposed quantum- classical hybrid. The result is extended to a constrained maximum with applications to integer programming and TSP (Traveling Salesman Problem).

A 2 × 2 quantum dot array with controllable inter-dot tunnel couplings

NASA Astrophysics Data System (ADS)

Mukhopadhyay, Uditendu; Dehollain, Juan Pablo; Reichl, Christian; Wegscheider, Werner; Vandersypen, Lieven M. K.

2018-04-01

The interaction between electrons in arrays of electrostatically defined quantum dots is naturally described by a Fermi-Hubbard Hamiltonian. Moreover, the high degree of tunability of these systems makes them a powerful platform to simulate different regimes of the Hubbard model. However, most quantum dot array implementations have been limited to one-dimensional linear arrays. In this letter, we present a square lattice unit cell of 2 × 2 quantum dots defined electrostatically in an AlGaAs/GaAs heterostructure using a double-layer gate technique. We probe the properties of the array using nearby quantum dots operated as charge sensors. We show that we can deterministically and dynamically control the charge occupation in each quantum dot in the single- to few-electron regime. Additionally, we achieve simultaneous individual control of the nearest-neighbor tunnel couplings over a range of 0-40 μeV. Finally, we demonstrate fast (˜1 μs) single-shot readout of the spin state of electrons in the dots through spin-to-charge conversion via Pauli spin blockade. These advances pave the way for analog quantum simulations in two dimensions, not previously accessible in quantum dot systems.

Computation of the properties of liquid neon, methane, and gas helium at low temperature by the Feynman-Hibbs approach.

PubMed

Tchouar, N; Ould-Kaddour, F; Levesque, D

2004-10-15

The properties of liquid methane, liquid neon, and gas helium are calculated at low temperatures over a large range of pressure from the classical molecular-dynamics simulations. The molecular interactions are represented by the Lennard-Jones pair potentials supplemented by quantum corrections following the Feynman-Hibbs approach. The equations of state, diffusion, and shear viscosity coefficients are determined for neon at 45 K, helium at 80 K, and methane at 110 K. A comparison is made with the existing experimental data and for thermodynamical quantities, with results computed from quantum numerical simulations when they are available. The theoretical variation of the viscosity coefficient with pressure is in good agreement with the experimental data when the quantum corrections are taken into account, thus reducing considerably the 60% discrepancy between the simulations and experiments in the absence of these corrections.

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.

Overcoming correlation fluctuations in two-photon interference experiments with differently bright and independently blinking remote quantum emitters

NASA Astrophysics Data System (ADS)

Weber, Jonas H.; Kettler, Jan; Vural, Hüseyin; Müller, Markus; Maisch, Julian; Jetter, Michael; Portalupi, Simone L.; Michler, Peter

2018-05-01

As a fundamental building block for quantum computation and communication protocols, the correct verification of the two-photon interference (TPI) contrast between two independent quantum light sources is of utmost importance. Here, we experimentally demonstrate how frequently present blinking dynamics and changes in emitter brightness critically affect the Hong-Ou-Mandel-type (HOM) correlation histograms of remote TPI experiments measured via the commonly utilized setup configuration. We further exploit this qualitative and quantitative explanation of the observed correlation dynamics to establish an alternative interferometer configuration, which is overcoming the discussed temporal fluctuations, giving rise to an error-free determination of the remote TPI visibility. We prove full knowledge of the obtained correlation by reproducing the measured correlation statistics via Monte Carlo simulations. As an exemplary system, we make use of two pairs of remote semiconductor quantum dots; however, the same conclusions apply for TPI experiments with flying qubits from any kind of remote solid-state quantum emitters.

Control of Multiple Exciton Generation and Electron-Phonon Coupling by Interior Nanospace in Hyperstructured Quantum Dot Superlattice.

PubMed

Chang, I-Ya; Kim, DaeGwi; Hyeon-Deuk, Kim

2017-09-20

The possibility of precisely manipulating interior nanospace, which can be adjusted by ligand-attaching down to the subnanometer regime, in a hyperstructured quantum dot (QD) superlattice (QDSL) induces a new kind of collective resonant coupling among QDs and opens up new opportunities for developing advanced optoelectric and photovoltaic devices. Here, we report the first real-time dynamics simulations of the multiple exciton generation (MEG) in one-, two-, and three-dimensional (1D, 2D, and 3D) hyperstructured H-passivated Si QDSLs, accounting for thermally fluctuating band energies and phonon dynamics obtained by finite-temperature ab initio molecular dynamics simulations. We computationally demonstrated that the MEG was significantly accelerated, especially in the 3D QDSL compared to the 1D and 2D QDSLs. The MEG acceleration in the 3D QDSL was almost 1.9 times the isolated QD case. The dimension-dependent MEG acceleration was attributed not only to the static density of states but also to the dynamical electron-phonon couplings depending on the dimensionality of the hyperstructured QDSL, which is effectively controlled by the interior nanospace. Such dimension-dependent modifications originated from the short-range quantum resonance among component QDs and were intrinsic to the hyperstructured QDSL. We propose that photoexcited dynamics including the MEG process can be effectively controlled by only manipulating the interior nanospace of the hyperstructured QDSL without changing component QD size, shape, compositions, ligand, etc.

Adiabatic quantum optimization for associative memory recall

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

Seddiqi, Hadayat; Humble, Travis S.

Hopfield networks are a variant of associative memory that recall patterns stored in the couplings of an Ising model. Stored memories are conventionally accessed as fixed points in the network dynamics that correspond to energetic minima of the spin state. We show that memories stored in a Hopfield network may also be recalled by energy minimization using adiabatic quantum optimization (AQO). Numerical simulations of the underlying quantum dynamics allow us to quantify AQO recall accuracy with respect to the number of stored memories and noise in the input key. We investigate AQO performance with respect to how memories are storedmore » in the Ising model according to different learning rules. Our results demonstrate that AQO recall accuracy varies strongly with learning rule, a behavior that is attributed to differences in energy landscapes. Consequently, learning rules offer a family of methods for programming adiabatic quantum optimization that we expect to be useful for characterizing AQO performance.« less

Adiabatic Quantum Optimization for Associative Memory Recall

NASA Astrophysics Data System (ADS)

Seddiqi, Hadayat; Humble, Travis

2014-12-01

Hopfield networks are a variant of associative memory that recall patterns stored in the couplings of an Ising model. Stored memories are conventionally accessed as fixed points in the network dynamics that correspond to energetic minima of the spin state. We show that memories stored in a Hopfield network may also be recalled by energy minimization using adiabatic quantum optimization (AQO). Numerical simulations of the underlying quantum dynamics allow us to quantify AQO recall accuracy with respect to the number of stored memories and noise in the input key. We investigate AQO performance with respect to how memories are stored in the Ising model according to different learning rules. Our results demonstrate that AQO recall accuracy varies strongly with learning rule, a behavior that is attributed to differences in energy landscapes. Consequently, learning rules offer a family of methods for programming adiabatic quantum optimization that we expect to be useful for characterizing AQO performance.

Adiabatic quantum optimization for associative memory recall

DOE PAGES

Seddiqi, Hadayat; Humble, Travis S.

2014-12-22

Hopfield networks are a variant of associative memory that recall patterns stored in the couplings of an Ising model. Stored memories are conventionally accessed as fixed points in the network dynamics that correspond to energetic minima of the spin state. We show that memories stored in a Hopfield network may also be recalled by energy minimization using adiabatic quantum optimization (AQO). Numerical simulations of the underlying quantum dynamics allow us to quantify AQO recall accuracy with respect to the number of stored memories and noise in the input key. We investigate AQO performance with respect to how memories are storedmore » in the Ising model according to different learning rules. Our results demonstrate that AQO recall accuracy varies strongly with learning rule, a behavior that is attributed to differences in energy landscapes. Consequently, learning rules offer a family of methods for programming adiabatic quantum optimization that we expect to be useful for characterizing AQO performance.« 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 Hash function and its application to privacy amplification in quantum key distribution, pseudo-random number generation and image encryption

NASA Astrophysics Data System (ADS)

Yang, Yu-Guang; Xu, Peng; Yang, Rui; Zhou, Yi-Hua; Shi, Wei-Min

2016-01-01

Quantum information and quantum computation have achieved a huge success during the last years. In this paper, we investigate the capability of quantum Hash function, which can be constructed by subtly modifying quantum walks, a famous quantum computation model. It is found that quantum Hash function can act as a hash function for the privacy amplification process of quantum key distribution systems with higher security. As a byproduct, quantum Hash function can also be used for pseudo-random number generation due to its inherent chaotic dynamics. Further we discuss the application of quantum Hash function to image encryption and propose a novel image encryption algorithm. Numerical simulations and performance comparisons show that quantum Hash function is eligible for privacy amplification in quantum key distribution, pseudo-random number generation and image encryption in terms of various hash tests and randomness tests. It extends the scope of application of quantum computation and quantum information.

Quantum Hash function and its application to privacy amplification in quantum key distribution, pseudo-random number generation and image encryption

PubMed Central

Yang, Yu-Guang; Xu, Peng; Yang, Rui; Zhou, Yi-Hua; Shi, Wei-Min

2016-01-01

Quantum information and quantum computation have achieved a huge success during the last years. In this paper, we investigate the capability of quantum Hash function, which can be constructed by subtly modifying quantum walks, a famous quantum computation model. It is found that quantum Hash function can act as a hash function for the privacy amplification process of quantum key distribution systems with higher security. As a byproduct, quantum Hash function can also be used for pseudo-random number generation due to its inherent chaotic dynamics. Further we discuss the application of quantum Hash function to image encryption and propose a novel image encryption algorithm. Numerical simulations and performance comparisons show that quantum Hash function is eligible for privacy amplification in quantum key distribution, pseudo-random number generation and image encryption in terms of various hash tests and randomness tests. It extends the scope of application of quantum computation and quantum information. PMID:26823196

Quantum Hash function and its application to privacy amplification in quantum key distribution, pseudo-random number generation and image encryption.

PubMed

Yang, Yu-Guang; Xu, Peng; Yang, Rui; Zhou, Yi-Hua; Shi, Wei-Min

2016-01-29

Quantum information and quantum computation have achieved a huge success during the last years. In this paper, we investigate the capability of quantum Hash function, which can be constructed by subtly modifying quantum walks, a famous quantum computation model. It is found that quantum Hash function can act as a hash function for the privacy amplification process of quantum key distribution systems with higher security. As a byproduct, quantum Hash function can also be used for pseudo-random number generation due to its inherent chaotic dynamics. Further we discuss the application of quantum Hash function to image encryption and propose a novel image encryption algorithm. Numerical simulations and performance comparisons show that quantum Hash function is eligible for privacy amplification in quantum key distribution, pseudo-random number generation and image encryption in terms of various hash tests and randomness tests. It extends the scope of application of quantum computation and quantum information.

Bit-level quantum color image encryption scheme with quantum cross-exchange operation and hyper-chaotic system

NASA Astrophysics Data System (ADS)

Zhou, Nanrun; Chen, Weiwei; Yan, Xinyu; Wang, Yunqian

2018-06-01

In order to obtain higher encryption efficiency, a bit-level quantum color image encryption scheme by exploiting quantum cross-exchange operation and a 5D hyper-chaotic system is designed. Additionally, to enhance the scrambling effect, the quantum channel swapping operation is employed to swap the gray values of corresponding pixels. The proposed color image encryption algorithm has larger key space and higher security since the 5D hyper-chaotic system has more complex dynamic behavior, better randomness and unpredictability than those based on low-dimensional hyper-chaotic systems. Simulations and theoretical analyses demonstrate that the presented bit-level quantum color image encryption scheme outperforms its classical counterparts in efficiency and security.

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

Computing Wigner distributions and time correlation functions using the quantum thermal bath method: application to proton transfer spectroscopy.

PubMed

Basire, Marie; Borgis, Daniel; Vuilleumier, Rodolphe

2013-08-14

Langevin dynamics coupled to a quantum thermal bath (QTB) allows for the inclusion of vibrational quantum effects in molecular dynamics simulations at virtually no additional computer cost. We investigate here the ability of the QTB method to reproduce the quantum Wigner distribution of a variety of model potentials, designed to assess the performances and limits of the method. We further compute the infrared spectrum of a multidimensional model of proton transfer in the gas phase and in solution, using classical trajectories sampled initially from the Wigner distribution. It is shown that for this type of system involving large anharmonicities and strong nonlinear coupling to the environment, the quantum thermal bath is able to sample the Wigner distribution satisfactorily and to account for both zero point energy and tunneling effects. It leads to quantum time correlation functions having the correct short-time behavior, and the correct associated spectral frequencies, but that are slightly too overdamped. This is attributed to the classical propagation approximation rather than the generation of the quantized initial conditions themselves.

Fast Implementation of Quantum Phase Gates and Creation of Cluster States via Transitionless Quantum Driving

NASA Astrophysics Data System (ADS)

Zhang, Chun-Ling; Liu, Wen-Wu

2018-05-01

In this paper, combining transitionless quantum driving and quantum Zeno dynamics, we propose an efficient scheme to fast implement a two-qubit quantum phase gate which can be used to generate cluster state of atoms trapped in distant cavities. The influence of various of various error sources including spontaneous emission and photon loss on the fidelity is analyzed via numerical simulation. The results show that this scheme not only takes less time than adiabatic scheme but also is not sensitive to both error sources. Additionally, a creation of N-atom cluster states is put forward as a typical example of the applications of the phase gates.

Simultaneous Bistability of a Qubit and Resonator in Circuit Quantum Electrodynamics

NASA Astrophysics Data System (ADS)

Mavrogordatos, Th. K.; Tancredi, G.; Elliott, M.; Peterer, M. J.; Patterson, A.; Rahamim, J.; Leek, P. J.; Ginossar, E.; Szymańska, M. H.

2017-01-01

We explore the joint activated dynamics exhibited by two quantum degrees of freedom: a cavity mode oscillator which is strongly coupled to a superconducting qubit in the strongly coherently driven dispersive regime. Dynamical simulations and complementary measurements show a range of parameters where both the cavity and the qubit exhibit sudden simultaneous switching between two metastable states. This manifests in ensemble averaged amplitudes of both the cavity and qubit exhibiting a partial coherent cancellation. Transmission measurements of driven microwave cavities coupled to transmon qubits show detailed features which agree with the theory in the regime of simultaneous switching.

Bifurcation-based adiabatic quantum computation with a nonlinear oscillator network

PubMed Central

Goto, Hayato

2016-01-01

The dynamics of nonlinear systems qualitatively change depending on their parameters, which is called bifurcation. A quantum-mechanical nonlinear oscillator can yield a quantum superposition of two oscillation states, known as a Schrödinger cat state, via quantum adiabatic evolution through its bifurcation point. Here we propose a quantum computer comprising such quantum nonlinear oscillators, instead of quantum bits, to solve hard combinatorial optimization problems. The nonlinear oscillator network finds optimal solutions via quantum adiabatic evolution, where nonlinear terms are increased slowly, in contrast to conventional adiabatic quantum computation or quantum annealing, where quantum fluctuation terms are decreased slowly. As a result of numerical simulations, it is concluded that quantum superposition and quantum fluctuation work effectively to find optimal solutions. It is also notable that the present computer is analogous to neural computers, which are also networks of nonlinear components. Thus, the present scheme will open new possibilities for quantum computation, nonlinear science, and artificial intelligence. PMID:26899997

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.

Combined quantum-mechanics/molecular-mechanics dynamics simulation of A-DNA double strands irradiated by ultra-low-energy carbon ions

NASA Astrophysics Data System (ADS)

Ngaojampa, C.; Nimmanpipug, P.; Yu, L. D.; Anuntalabhochai, S.; Lee, V. S.

2011-02-01

In order to promote understanding of the fundamentals of ultra-low-energy ion interaction with DNA, molecular dynamics simulations using combined quantum-mechanics/molecular-mechanics of poly-AT and poly-GC A-DNA double strands irradiated by <200 eV carbon ions were performed to investigate the molecular implications of mutation bias. The simulations were focused on the responses of the DNA backbones and nitrogenous bases to irradiation. Analyses of the root mean square displacements of the backbones and non-hydrogen atoms of base rings of the simulated DNA structure after irradiation revealed a potential preference of DNA double strand separation, dependent on the irradiating energy. The results show that for the backbones, the large difference in the displacement between poly-GC and poly-AT in the initial time period could be the reason for the backbone breakage; for the nitrogenous base pairs, A-T is 30% more sensitive or vulnerable to ion irradiation than G-C, demonstrating a preferential, instead of random, effect of irradiation-induced mutation.

Parallel Decomposition of the Fictitious Lagrangian Algorithm and its Accuracy for Molecular Dynamics Simulations of Semiconductors.

NASA Astrophysics Data System (ADS)

Yeh, Mei-Ling

We have performed a parallel decomposition of the fictitious Lagrangian method for molecular dynamics with tight-binding total energy expression into the hypercube computer. This is the first time in literature that the dynamical simulation of semiconducting systems containing more than 512 silicon atoms has become possible with the electrons treated as quantum particles. With the utilization of the Intel Paragon system, our timing analysis predicts that our code is expected to perform realistic simulations on very large systems consisting of thousands of atoms with time requirements of the order of tens of hours. Timing results and performance analysis of our parallel code are presented in terms of calculation time, communication time, and setup time. The accuracy of the fictitious Lagrangian method in molecular dynamics simulation is also investigated, especially the energy conservation of the total energy of ions. We find that the accuracy of the fictitious Lagrangian scheme in small silicon cluster and very large silicon system simulations is good for as long as the simulations proceed, even though we quench the electronic coordinates to the Born-Oppenheimer surface only in the beginning of the run. The kinetic energy of electrons does not increase as time goes on, and the energy conservation of the ionic subsystem remains very good. This means that, as far as the ionic subsystem is concerned, the electrons are on the average in the true quantum ground states. We also tie up some odds and ends regarding a few remaining questions about the fictitious Lagrangian method, such as the difference between the results obtained from the Gram-Schmidt and SHAKE method of orthonormalization, and differences between simulations where the electrons are quenched to the Born -Oppenheimer surface only once compared with periodic quenching.

Mass Transport in the Warm, Dense Matter and High-Energy Density Regimes

NASA Astrophysics Data System (ADS)

Kress, J. D.; Burakovsky, L.; Ticknor, C.; Collins, L. A.; Lambert, F.

2011-10-01

Large-scale hydrodynamical simulations of fluids and plasmas under extreme conditions require knowledge of certain microscopic properties such as diffusion and viscosity in addition to the equation-of-state. To determine these dynamical properties, we employ quantum molecular dynamical (MD) simulations on large samples of atoms. The method has several advantages: 1) static, dynamical, and optical properties are produced consistently from the same simulations, and 2) mixture properties arise in a natural way since all intra- and inter-particle interactions are properly represented. We utilize two forms of density functional theory: 1) Kohn-Sham (KS-DFT) and 2) orbital-free (OF-DFT). KS-DFT is computationally intense due to its reliance on an orbital representation. As the temperature rises, the Thomas-Fermi approximation in OF-DFT begins to represent accurately the density functional, and provides an efficient and systematic means for extending the quantum simulations to very hot conditions. We have performed KS-DFT and OF-DFT calculations of the self-diffusion, mutual diffusion and shear viscosity for Al, Li, H, and LiH. We examine trends in these quantities and compare to more approximate forms such as the one-component plasma model. We also determine the validity of mixing rules that combine the properties of pure species into a composite result.

Supramolecular polymerization of benzene-1,3,5-tricarboxamide: a molecular dynamics simulation study.

PubMed

Bejagam, Karteek K; Fiorin, Giacomo; Klein, Michael L; Balasubramanian, Sundaram

2014-05-15

Supramolecular polymerization in the family of benzene-1,3,5-tricarboxamide (BTA) has been investigated using atomistic molecular dynamics (MD) simulations. Gas phase calculations using a nonpolarizable force field reproduce the cooperativity in binding energy and intermolecular structure seen in quantum chemical calculations. Both quantum chemical and force field based calculations suggest that the ground state structure of the BTA dimer contains two donor hydrogen bonds and one acceptor hydrogen bond rather than the conjectured three-donor and zero-acceptor hydrogen-bonded state. MD simulations of BTA molecules in a realistic solvent, n-nonane, demonstrate the self-assembly process. The free energy (FE) of dimerization and of solvation has been determined. The solvated dimer of BTA with hexyl tails is more stable than two monomers by about 13 kcal/mol. Furthermore, the FE of association of a BTA molecule to an oligomer exhibits a dependence on the oligomer size, which is a robust signature of cooperative self-assembly.

Semiclassical Monte Carlo: A first principles approach to non-adiabatic molecular dynamics

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

White, Alexander J.; Center for Nonlinear Studies; Gorshkov, Vyacheslav N.

2014-11-14

Modeling the dynamics of photophysical and (photo)chemical reactions in extended molecular systems is a new frontier for quantum chemistry. Many dynamical phenomena, such as intersystem crossing, non-radiative relaxation, and charge and energy transfer, require a non-adiabatic description which incorporate transitions between electronic states. Additionally, these dynamics are often highly sensitive to quantum coherences and interference effects. Several methods exist to simulate non-adiabatic dynamics; however, they are typically either too expensive to be applied to large molecular systems (10's-100's of atoms), or they are based on ad hoc schemes which may include severe approximations due to inconsistencies in classical and quantummore » mechanics. We present, in detail, an algorithm based on Monte Carlo sampling of the semiclassical time-dependent wavefunction that involves running simple surface hopping dynamics, followed by a post-processing step which adds little cost. The method requires only a few quantities from quantum chemistry calculations, can systematically be improved, and provides excellent agreement with exact quantum mechanical results. Here we show excellent agreement with exact solutions for scattering results of standard test problems. Additionally, we find that convergence of the wavefunction is controlled by complex valued phase factors, the size of the non-adiabatic coupling region, and the choice of sampling function. These results help in determining the range of applicability of the method, and provide a starting point for further improvement.« less

Application of quantum master equation for long-term prognosis of asset-prices

NASA Astrophysics Data System (ADS)

Khrennikova, Polina

2016-05-01

This study combines the disciplines of behavioral finance and an extension of econophysics, namely the concepts and mathematical structure of quantum physics. We apply the formalism of quantum theory to model the dynamics of some correlated financial assets, where the proposed model can be potentially applied for developing a long-term prognosis of asset price formation. At the informational level, the asset price states interact with each other by the means of a ;financial bath;. The latter is composed of agents' expectations about the future developments of asset prices on the finance market, as well as financially important information from mass-media, society, and politicians. One of the essential behavioral factors leading to the quantum-like dynamics of asset prices is the irrationality of agents' expectations operating on the finance market. These expectations lead to a deeper type of uncertainty concerning the future price dynamics of the assets, than given by a classical probability theory, e.g., in the framework of the classical financial mathematics, which is based on the theory of stochastic processes. The quantum dimension of the uncertainty in price dynamics is expressed in the form of the price-states superposition and entanglement between the prices of the different financial assets. In our model, the resolution of this deep quantum uncertainty is mathematically captured with the aid of the quantum master equation (its quantum Markov approximation). We illustrate our model of preparation of a future asset price prognosis by a numerical simulation, involving two correlated assets. Their returns interact more intensively, than understood by a classical statistical correlation. The model predictions can be extended to more complex models to obtain price configuration for multiple assets and portfolios.

Theoretical study of dynamic electron-spin-polarization via the doublet-quartet quantum-mixed state and time-resolved ESR spectra of the quartet high-spin state.

PubMed

Teki, Yoshio; Matsumoto, Takafumi

2011-04-07

The mechanism of the unique dynamic electron polarization of the quartet (S = 3/2) high-spin state via a doublet-quartet quantum-mixed state and detail theoretical calculations of the population transfer are reported. By the photo-induced electron transfer, the quantum-mixed charge-separate state is generated in acceptor-donor-radical triad (A-D-R). This mechanism explains well the unique dynamic electron polarization of the quartet state of A-D-R. The generation of the selectively populated quantum-mixed state and its transfer to the strongly coupled pure quartet and doublet states have been treated both by a perturbation approach and by exact numerical calculations. The analytical solutions show that generation of the quantum-mixed states with the selective populations after de-coherence and/or accompanying the (complete) dephasing during the charge-recombination are essential for the unique dynamic electron polarization. Thus, the elimination of the quantum coherence (loss of the quantum information) is the key process for the population transfer from the quantum-mixed state to the quartet state. The generation of high-field polarization on the strongly coupled quartet state by the charge-recombination process can be explained by a polarization transfer from the quantum-mixed charge-separate state. Typical time-resolved ESR patterns of the quantum-mixed state and of the strongly coupled quartet state are simulated based on the generation mechanism of the dynamic electron polarization. The dependence of the spectral pattern of the quartet high-spin state has been clarified for the fine-structure tensor and the exchange interaction of the quantum-mixed state. The spectral pattern of the quartet state is not sensitive towards the fine-structure tensor of the quantum-mixed state, because this tensor contributes only as a perturbation in the population transfer to the spin-sublevels of the quartet state. Based on the stochastic Liouville equation, it is also discussed why the selective population in the quantum-mixed state is generated for the "finite field" spin-sublevels. The numerical calculations of the elimination of the quantum coherence (de-coherence and/or dephasing) are demonstrated. A new possibility of the enhanced intersystem crossing pathway in solution is also proposed.

Density functional theory calculation of refractive indices of liquid-forming silicon oil compounds

NASA Astrophysics Data System (ADS)

Lee, Sanghun; Park, Sung Soo; Hagelberg, Frank

2012-02-01

A combination of quantum chemical calculation and molecular dynamics simulation is applied to compute refractive indices of liquid-forming silicon oils. The densities of these species are obtained from molecular dynamics simulations based on the NPT ensemble while the molecular polarizabilities are evaluated by density functional theory. This procedure is shown to yield results well compatible with available experimental data, suggesting that it represents a robust and economic route for determining the refractive indices of liquid-forming organic complexes containing silicon.

A Direct, Quantitative Connection between Molecular Dynamics Simulations and Vibrational Probe Line Shapes.

PubMed

Xu, Rosalind J; Blasiak, Bartosz; Cho, Minhaeng; Layfield, Joshua P; Londergan, Casey H

2018-05-17

A quantitative connection between molecular dynamics simulations and vibrational spectroscopy of probe-labeled systems would enable direct translation of experimental data into structural and dynamical information. To constitute this connection, all-atom molecular dynamics (MD) simulations were performed for two SCN probe sites (solvent-exposed and buried) in a calmodulin-target peptide complex. Two frequency calculation approaches with substantial nonelectrostatic components, a quantum mechanics/molecular mechanics (QM/MM)-based technique and a solvatochromic fragment potential (SolEFP) approach, were used to simulate the infrared probe line shapes. While QM/MM results disagreed with experiment, SolEFP results matched experimental frequencies and line shapes and revealed the physical and dynamic bases for the observed spectroscopic behavior. The main determinant of the CN probe frequency is the exchange repulsion between the probe and its local structural neighbors, and there is a clear dynamic explanation for the relatively broad probe line shape observed at the "buried" probe site. This methodology should be widely applicable to vibrational probes in many environments.

Multiscale Aspects of Modeling Gas-Phase Nanoparticle Synthesis

PubMed Central

Buesser, B.; Gröhn, A.J.

2013-01-01

Aerosol reactors are utilized to manufacture nanoparticles in industrially relevant quantities. The development, understanding and scale-up of aerosol reactors can be facilitated with models and computer simulations. This review aims to provide an overview of recent developments of models and simulations and discuss their interconnection in a multiscale approach. A short introduction of the various aerosol reactor types and gas-phase particle dynamics is presented as a background for the later discussion of the models and simulations. Models are presented with decreasing time and length scales in sections on continuum, mesoscale, molecular dynamics and quantum mechanics models. PMID:23729992

Lenard-Balescu calculations and classical molecular dynamics simulations of electrical and thermal conductivities of hydrogen plasmas

DOE PAGES

Whitley, Heather D.; Scullard, Christian R.; Benedict, Lorin X.; ...

2014-12-04

Here, we present a discussion of kinetic theory treatments of linear electrical and thermal transport in hydrogen plasmas, for a regime of interest to inertial confinement fusion applications. In order to assess the accuracy of one of the more involved of these approaches, classical Lenard-Balescu theory, we perform classical molecular dynamics simulations of hydrogen plasmas using 2-body quantum statistical potentials and compute both electrical and thermal conductivity from out particle trajectories using the Kubo approach. Our classical Lenard-Balescu results employing the identical statistical potentials agree well with the simulations.

Nuclear quantum effects in electronically adiabatic quantum time correlation functions: Application to the absorption spectrum of a hydrated electron

NASA Astrophysics Data System (ADS)

Turi, László; Hantal, György; Rossky, Peter J.; Borgis, Daniel

2009-07-01

A general formalism for introducing nuclear quantum effects in the expression of the quantum time correlation function of an operator in a multilevel electronic system is presented in the adiabatic limit. The final formula includes the nuclear quantum time correlation functions of the operator matrix elements, of the energy gap, and their cross terms. These quantities can be inferred and evaluated from their classical analogs obtained by mixed quantum-classical molecular dynamics simulations. The formalism is applied to the absorption spectrum of a hydrated electron, expressed in terms of the time correlation function of the dipole operator in the ground electronic state. We find that both static and dynamic nuclear quantum effects distinctly influence the shape of the absorption spectrum, especially its high energy tail related to transitions to delocalized electron states. Their inclusion does improve significantly the agreement between theory and experiment for both the low and high frequency edges of the spectrum. It does not appear sufficient, however, to resolve persistent deviations in the slow Lorentzian-like decay part of the spectrum in the intermediate 2-3 eV region.

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

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

Ulusoy, Inga S.; Center for Computational and Molecular Science and Technology, School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, Georgia 30332-0400; Andrienko, Daniil A.

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

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

NASA Astrophysics Data System (ADS)

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

2016-06-01

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

Quantum-assisted biomolecular modelling.

PubMed

Harris, Sarah A; Kendon, Vivien M

2010-08-13

Our understanding of the physics of biological molecules, such as proteins and DNA, is limited because the approximations we usually apply to model inert materials are not, in general, applicable to soft, chemically inhomogeneous systems. The configurational complexity of biomolecules means the entropic contribution to the free energy is a significant factor in their behaviour, requiring detailed dynamical calculations to fully evaluate. Computer simulations capable of taking all interatomic interactions into account are therefore vital. However, even with the best current supercomputing facilities, we are unable to capture enough of the most interesting aspects of their behaviour to properly understand how they work. This limits our ability to design new molecules, to treat diseases, for example. Progress in biomolecular simulation depends crucially on increasing the computing power available. Faster classical computers are in the pipeline, but these provide only incremental improvements. Quantum computing offers the possibility of performing huge numbers of calculations in parallel, when it becomes available. We discuss the current open questions in biomolecular simulation, how these might be addressed using quantum computation and speculate on the future importance of quantum-assisted biomolecular modelling.

Quantum Dynamics of Solitons in Strongly Interacting Systems on Optical Lattices

NASA Astrophysics Data System (ADS)

Rubbo, Chester; Balakrishnan, Radha; Reinhardt, William; Satija, Indubala; Rey, Ana; Manmana, Salvatore

2012-06-01

We present results of the quantum dynamics of solitons in XXZ spin-1/2 systems which in general can be derived from a system of spinless fermions or hard-core bosons (HCB) with nearest neighbor interaction on a lattice. A mean-field treatment using spin-coherent states revealed analytic solutions of both bright and dark solitons [1]. We take these solutions and apply a full quantum evolution using the adaptive time-dependent density matrix renormalization group method (adaptive t-DMRG), which takes into account the effect of strong correlations. We use local spin observables, correlations functions, and entanglement entropies as measures for the stability of these soliton solutions over the simulation times. [4pt] [1] R. Balakrishnan, I.I. Satija, and C.W. Clark, Phys. Rev. Lett. 103, 230403 (2009).

Effects of two-photon absorption on all optical logic operation based on quantum-dot semiconductor optical amplifiers

NASA Astrophysics Data System (ADS)

Zhang, Xiang; Dutta, Niloy K.

2018-01-01

We investigate all-optical logic operation in quantum-dot semiconductor optical amplifier (QD-SOA) based Mach-Zehnder interferometer considering the effects of two-photon absorption (TPA). TPA occurs during the propagation of sub-picosecond pulses in QD-SOA, which leads to a change in carrier recovery dynamics in quantum-dots. We utilize a rate equation model to take into account carrier refill through TPA and nonlinear dynamics including carrier heating and spectral hole burning in the QD-SOA. The simulation results show the TPA-induced pumping in the QD-SOA can reduce the pattern effect and increase the output quality of the all-optical logic operation. With TPA, this scheme is suitable for high-speed Boolean logic operation at 320 Gb/s.

Ultrafast dynamics induced by the interaction of molecules with electromagnetic fields: Several quantum, semiclassical, and classical approaches.

PubMed

Antipov, Sergey V; Bhattacharyya, Swarnendu; El Hage, Krystel; Xu, Zhen-Hao; Meuwly, Markus; Rothlisberger, Ursula; Vaníček, Jiří

2017-11-01

Several strategies for simulating the ultrafast dynamics of molecules induced by interactions with electromagnetic fields are presented. After a brief overview of the theory of molecule-field interaction, we present several representative examples of quantum, semiclassical, and classical approaches to describe the ultrafast molecular dynamics, including the multiconfiguration time-dependent Hartree method, Bohmian dynamics, local control theory, semiclassical thawed Gaussian approximation, phase averaging, dephasing representation, molecular mechanics with proton transfer, and multipolar force fields. In addition to the general overview, some focus is given to the description of nuclear quantum effects and to the direct dynamics, in which the ab initio energies and forces acting on the nuclei are evaluated on the fly. Several practical applications, performed within the framework of the Swiss National Center of Competence in Research "Molecular Ultrafast Science and Technology," are presented: These include Bohmian dynamics description of the collision of H with H 2 , local control theory applied to the photoinduced ultrafast intramolecular proton transfer, semiclassical evaluation of vibrationally resolved electronic absorption, emission, photoelectron, and time-resolved stimulated emission spectra, infrared spectroscopy of H-bonding systems, and multipolar force fields applications in the condensed phase.

Ultrafast dynamics induced by the interaction of molecules with electromagnetic fields: Several quantum, semiclassical, and classical approaches

PubMed Central

Antipov, Sergey V.; Bhattacharyya, Swarnendu; El Hage, Krystel; Xu, Zhen-Hao; Meuwly, Markus; Rothlisberger, Ursula; Vaníček, Jiří

2018-01-01

Several strategies for simulating the ultrafast dynamics of molecules induced by interactions with electromagnetic fields are presented. After a brief overview of the theory of molecule-field interaction, we present several representative examples of quantum, semiclassical, and classical approaches to describe the ultrafast molecular dynamics, including the multiconfiguration time-dependent Hartree method, Bohmian dynamics, local control theory, semiclassical thawed Gaussian approximation, phase averaging, dephasing representation, molecular mechanics with proton transfer, and multipolar force fields. In addition to the general overview, some focus is given to the description of nuclear quantum effects and to the direct dynamics, in which the ab initio energies and forces acting on the nuclei are evaluated on the fly. Several practical applications, performed within the framework of the Swiss National Center of Competence in Research “Molecular Ultrafast Science and Technology,” are presented: These include Bohmian dynamics description of the collision of H with H2, local control theory applied to the photoinduced ultrafast intramolecular proton transfer, semiclassical evaluation of vibrationally resolved electronic absorption, emission, photoelectron, and time-resolved stimulated emission spectra, infrared spectroscopy of H-bonding systems, and multipolar force fields applications in the condensed phase. PMID:29376107

Nonlinear low-frequency electrostatic wave dynamics in a two-dimensional quantum plasma

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

Ghosh, Samiran, E-mail: sran_g@yahoo.com; Chakrabarti, Nikhil, E-mail: nikhil.chakrabarti@saha.ac.in

2016-08-15

The problem of two-dimensional arbitrary amplitude low-frequency electrostatic oscillation in a quasi-neutral quantum plasma is solved exactly by elementary means. In such quantum plasmas we have treated electrons quantum mechanically and ions classically. The exact analytical solution of the nonlinear system exhibits the formation of dark and black solitons. Numerical simulation also predicts the possible periodic solution of the nonlinear system. Nonlinear analysis reveals that the system does have a bifurcation at a critical Mach number that depends on the angle of propagation of the wave. The small-amplitude limit leads to the formation of weakly nonlinear Kadomstev–Petviashvili solitons.

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 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.

Quantumness-generating capability of quantum dynamics

NASA Astrophysics Data System (ADS)

Li, Nan; Luo, Shunlong; Mao, Yuanyuan

2018-04-01

We study quantumness-generating capability of quantum dynamics, where quantumness refers to the noncommutativity between the initial state and the evolving state. In terms of the commutator of the square roots of the initial state and the evolving state, we define a measure to quantify the quantumness-generating capability of quantum dynamics with respect to initial states. Quantumness-generating capability is absent in classical dynamics and hence is a fundamental characteristic of quantum dynamics. For qubit systems, we present an analytical form for this measure, by virtue of which we analyze several prototypical dynamics such as unitary dynamics, phase damping dynamics, amplitude damping dynamics, and random unitary dynamics (Pauli channels). Necessary and sufficient conditions for the monotonicity of quantumness-generating capability are also identified. Finally, we compare these conditions for the monotonicity of quantumness-generating capability with those for various Markovianities and illustrate that quantumness-generating capability and quantum Markovianity are closely related, although they capture different aspects of quantum dynamics.

Impact of geometric, thermal and tunneling effects on nano-transistors

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

Hu, Langhua; Chen, Duan, E-mail: dchen10@uncc.edu; Wei, Guo-Wei

Electronic transistors are fundamental building blocks of large scale integrated circuits in modern advanced electronic equipments, and their sizes have been down-scaled to nanometers. Modeling and simulations in the framework of quantum dynamics have emerged as important tools to study functional characteristics of these nano-devices. This work explores the effects of geometric shapes of semiconductor–insulator interfaces, phonon–electron interactions, and quantum tunneling of three-dimensional (3D) nano-transistors. First, we propose a two-scale energy functional to describe the electron dynamics in a dielectric continuum of device material. Coupled governing equations, i.e., Poisson–Kohn–Sham (PKS) equations, are derived by the variational principle. Additionally, it ismore » found that at a given channel cross section area and gate voltage, the geometry that has the smallest perimeter of the channel cross section offers the largest channel current, which indicates that ultra-thin nanotransistors may not be very efficient in practical applications. Moreover, we introduce a new method to evaluate quantum tunneling effects in nanotransistors without invoking the comparison of classical and quantum predictions. It is found that at a given channel cross section area and gate voltage, the geometry that has the smallest perimeter of the channel cross section has the smallest quantum tunneling ratio, which indicates that geometric defects can lead to higher geometric confinement and larger quantum tunneling effect. Furthermore, although an increase in the phonon–electron interaction strength reduces channel current, it does not have much impact to the quantum tunneling ratio. Finally, advanced numerical techniques, including second order elliptic interface methods, have been applied to ensure computational accuracy and reliability of the present PKS simulation.« less

Non-equilibrium dynamics of artificial quantum matter

NASA Astrophysics Data System (ADS)

Babadi, Mehrtash

The rapid progress of the field of ultracold atoms during the past two decades has set new milestones in our control over matter. By cooling dilute atomic gases and molecules to nano-Kelvin temperatures, novel quantum mechanical states of matter can be realized and studied on a table-top experimental setup while bulk matter can be tailored to faithfully simulate abstract theoretical models. Two of such models which have witnessed significant experimental and theoretical attention are (1) the two-component Fermi gas with resonant s-wave interactions, and (2) the single-component Fermi gas with dipole-dipole interactions. This thesis is devoted to studying the non-equilibrium collective dynamics of these systems using the general framework of quantum kinetic theory. We present a concise review of the utilized mathematical methods in the first two chapters, including the Schwinger-Keldysh formalism of non-equilibrium quantum fields, two-particle irreducible (2PI) effective actions and the framework of quantum kinetic theory. We study the collective dynamics of the dipolar Fermi gas in a quasi-two-dimensional optical trap in chapter 3 and provide a detailed account of its dynamical crossover from the collisionless to the hydrodynamical regime. Chapter 4 is devoted to studying the dynamics of the attractive Fermi gas in the normal phase. Starting from the self-consistent T-matrix (pairing fluctuation) approximation, we systematically derive a set of quantum kinetic equations and show that they provide a globally valid description of the dynamics of the attractive Fermi gas, ranging from the weak-coupling Fermi liquid phase to the intermediate non-Fermi liquid pairing pseudogap regime and finally the strong-coupling Bose liquid phase. The shortcomings of the self-consistent T-matrix approximation in two spatial dimensions are discussed along with a proposal to overcome its unphysical behaviors. The developed kinetic formalism is finally utilized to reproduce and interpret the findings of a recent experiment done on the collective dynamics of trapped two-dimensional ultracold gases.

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 framework for stochastic simulations and visualization of biological electron-transfer dynamics

NASA Astrophysics Data System (ADS)

Nakano, C. Masato; Byun, Hye Suk; Ma, Heng; Wei, Tao; El-Naggar, Mohamed Y.

2015-08-01

Electron transfer (ET) dictates a wide variety of energy-conversion processes in biological systems. Visualizing ET dynamics could provide key insight into understanding and possibly controlling these processes. We present a computational framework named VizBET to visualize biological ET dynamics, using an outer-membrane Mtr-Omc cytochrome complex in Shewanella oneidensis MR-1 as an example. Starting from X-ray crystal structures of the constituent cytochromes, molecular dynamics simulations are combined with homology modeling, protein docking, and binding free energy computations to sample the configuration of the complex as well as the change of the free energy associated with ET. This information, along with quantum-mechanical calculations of the electronic coupling, provides inputs to kinetic Monte Carlo (KMC) simulations of ET dynamics in a network of heme groups within the complex. Visualization of the KMC simulation results has been implemented as a plugin to the Visual Molecular Dynamics (VMD) software. VizBET has been used to reveal the nature of ET dynamics associated with novel nonequilibrium phase transitions in a candidate configuration of the Mtr-Omc complex due to electron-electron interactions.

A quantum dynamics study of the benzopyran ring opening guided by laser pulses

NASA Astrophysics Data System (ADS)

Saab, Mohamad; Doriol, Loïc Joubert; Lasorne, Benjamin; Guérin, Stéphane; Gatti, Fabien

2014-10-01

The ring-opening photoisomerization of benzopyran, which occurs via a photochemical route involving a conical intersection, has been studied with quantum dynamics calculations using the multi-configuration time-dependent Hartree method (MCTDH). We introduce a mechanistic strategy to control the conversion of benzopyran to merocyanine with laser pulses. We use a six-dimensional model developed in a previous work for the potential energy surfaces (PES) based on an extension of the vibronic-coupling Hamiltonian model (diabatization method by ansatz), which depends on the most active degrees of freedom. The main objective of these quantum dynamics simulations is to provide a set of strategies that could help experimentalists to control the photoreactivity vs. photostability ratio (selectivity). In this work we present: (i) a pump-dump technique used to control the photostability, (ii) a two-step strategy to enhance the reactivity of the system: first, a pure vibrational excitation in the electronic ground state that prepares the system and, second, an ultraviolet excitation that brings the system to the first adiabatic electronic state; (iii) finally the effect of a non-resonant pulse (Stark effect) on the dynamics.

Cooperating or fighting with control noise in the optimal manipulation of quantum dynamics

NASA Astrophysics Data System (ADS)

Shuang, Feng; Rabitz, Herschel

2004-11-01

This paper investigates the impact of control field noise on the optimal manipulation of quantum dynamics. Simulations are performed on several multilevel quantum systems with the goal of population transfer in the presence of significant control noise. The noise enters as run-to-run variations in the control amplitude and phase with the observation being an ensemble average over many runs as is commonly done in the laboratory. A genetic algorithm with an improved elitism operator is used to find the optimal field that either fights against or cooperates with control field noise. When seeking a high control yield it is possible to find fields that successfully fight with the noise while attaining good quality stable results. When seeking modest control yields, fields can be found which are optimally shaped to cooperate with the noise and thereby drive the dynamics more efficiently. In general, noise reduces the coherence of the dynamics, but the results indicate that population transfer objectives can be met by appropriately either fighting or cooperating with noise, even when it is intense.

Cooperating or fighting with control noise in the optimal manipulation of quantum dynamics.

PubMed

Shuang, Feng; Rabitz, Herschel

2004-11-15

This paper investigates the impact of control field noise on the optimal manipulation of quantum dynamics. Simulations are performed on several multilevel quantum systems with the goal of population transfer in the presence of significant control noise. The noise enters as run-to-run variations in the control amplitude and phase with the observation being an ensemble average over many runs as is commonly done in the laboratory. A genetic algorithm with an improved elitism operator is used to find the optimal field that either fights against or cooperates with control field noise. When seeking a high control yield it is possible to find fields that successfully fight with the noise while attaining good quality stable results. When seeking modest control yields, fields can be found which are optimally shaped to cooperate with the noise and thereby drive the dynamics more efficiently. In general, noise reduces the coherence of the dynamics, but the results indicate that population transfer objectives can be met by appropriately either fighting or cooperating with noise, even when it is intense.

Deuteration as a Means to Tune Crystallinity of Conducting Polymers

DOE PAGES

Jakowski, Jacek; Huang, Jingsong; Garashchuk, Sophya; ...

2017-08-25

The effects of deuterium isotope substitution on conjugated polymer chain stacking of poly(3-hexylthiophene) is studied in this paper experimentally by X-ray diffraction (XRD) in combination with gel permeation chromatography and theoretically using density functional theory and quantum molecular dynamics. For four P3HT materials with different levels of deuteration (pristine, main-chain deuterated, side-chain deuterated, and fully deuterated), the XRD measurements show that main-chain thiophene deuteration significantly reduces crystallinity, regardless of the side-chain deuteration. The reduction of crystallinity due to the main-chain deuteration is a quantum nuclear effect resulting from a static zero-point vibrational energy combined with a dynamic correlation of themore » dipole fluctuations. The quantum molecular dynamics simulations confirm the interchain correlation of the proton–proton and deuteron–deuteron motions but not of the proton–deuteron motion. Thus and finally, isotopic purity is an important factor affecting stability and properties of conjugated polymer crystals, which should be considered in the design of electronic and spintronic devices.« less

Higher-order stochastic differential equations and the positive Wigner function

NASA Astrophysics Data System (ADS)

Drummond, P. D.

2017-12-01

General higher-order stochastic processes that correspond to any diffusion-type tensor of higher than second order are obtained. The relationship of multivariate higher-order stochastic differential equations with tensor decomposition theory and tensor rank is explained. Techniques for generating the requisite complex higher-order noise are proved to exist either using polar coordinates and γ distributions, or from products of Gaussian variates. This method is shown to allow the calculation of the dynamics of the Wigner function, after it is extended to a complex phase space. The results are illustrated physically through dynamical calculations of the positive Wigner distribution for three-mode parametric downconversion, widely used in quantum optics. The approach eliminates paradoxes arising from truncation of the higher derivative terms in Wigner function time evolution. Anomalous results of negative populations and vacuum scattering found in truncated Wigner quantum simulations in quantum optics and Bose-Einstein condensate dynamics are shown not to occur with this type of stochastic theory.

Deuteration as a Means to Tune Crystallinity of Conducting Polymers

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

Jakowski, Jacek; Huang, Jingsong; Garashchuk, Sophya

The effects of deuterium isotope substitution on conjugated polymer chain stacking of poly(3-hexylthiophene) is studied in this paper experimentally by X-ray diffraction (XRD) in combination with gel permeation chromatography and theoretically using density functional theory and quantum molecular dynamics. For four P3HT materials with different levels of deuteration (pristine, main-chain deuterated, side-chain deuterated, and fully deuterated), the XRD measurements show that main-chain thiophene deuteration significantly reduces crystallinity, regardless of the side-chain deuteration. The reduction of crystallinity due to the main-chain deuteration is a quantum nuclear effect resulting from a static zero-point vibrational energy combined with a dynamic correlation of themore » dipole fluctuations. The quantum molecular dynamics simulations confirm the interchain correlation of the proton–proton and deuteron–deuteron motions but not of the proton–deuteron motion. Thus and finally, isotopic purity is an important factor affecting stability and properties of conjugated polymer crystals, which should be considered in the design of electronic and spintronic devices.« less

Chain representations of Open Quantum Systems and Lieb-Robinson like bounds for the dynamics

NASA Astrophysics Data System (ADS)

Woods, Mischa

2013-03-01

This talk is concerned with the mapping of the Hamiltonian of open quantum systems onto chain representations, which forms the basis for a rigorous theory of the interaction of a system with its environment. This mapping progresses as an interaction which gives rise to a sequence of residual spectral densities of the system. The rigorous mathematical properties of this mapping have been unknown so far. Here we develop the theory of secondary measures to derive an analytic, expression for the sequence solely in terms of the initial measure and its associated orthogonal polynomials of the first and second kind. These mappings can be thought of as taking a highly nonlocal Hamiltonian to a local Hamiltonian. In the latter, a Lieb-Robinson like bound for the dynamics of the open quantum system makes sense. We develop analytical bounds on the error to observables of the system as a function of time when the semi-infinite chain in truncated at some finite length. The fact that this is possible shows that there is a finite ``Speed of sound'' in these chain representations. This has many implications of the simulatability of open quantum systems of this type and demonstrates that a truncated chain can faithfully reproduce the dynamics at shorter times. These results make a significant and mathematically rigorous contribution to the understanding of the theory of open quantum systems; and pave the way towards the efficient simulation of these systems, which within the standard methods, is often an intractable problem. EPSRC CDT in Controlled Quantum Dynamics, EU STREP project and Alexander von Humboldt Foundation

Symmetrical windowing for quantum states in quasi-classical trajectory simulations: Application to electronically non-adiabatic processes

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

Cotton, Stephen J.; Miller, William H., E-mail: millerwh@berkeley.edu

A recently described symmetrical windowing methodology [S. J. Cotton and W. H. Miller, J. Phys. Chem. A 117, 7190 (2013)] for quasi-classical trajectory simulations is applied here to the Meyer-Miller [H.-D. Meyer and W. H. Miller, J. Chem. Phys. 70, 3214 (1979)] model for the electronic degrees of freedom in electronically non-adiabatic dynamics. Results generated using this classical approach are observed to be in very good agreement with accurate quantum mechanical results for a variety of test applications, including problems where coherence effects are significant such as the challenging asymmetric spin-boson system.

Nuclear quantum fluctuations in ice I(h).

PubMed

Moreira, Pedro Augusto Franco Pinheiro; de Koning, Maurice

2015-10-14

We discuss the role of nuclear quantum fluctuations in ice Ih, focusing on the hydrogen-bond (HB) structure and the molecular dipole-moment distribution. For this purpose we carry out DFT-based first-principles molecular dynamics and path-integral molecular dynamics simulations at T = 100 K. We analyze the HB structure in terms of a set of parameters previously employed to characterize molecular structures in the liquid phase and compute the molecular dipole moments using the maximally-localized Wannier functions. The results show that the protons experience very large digressions driven by quantum fluctuations, accompanied by major rearrangements in the electronic density. As a result of these protonic quantum fluctuations the molecular dipole-moment distribution is substantially broadened as well as shifted to a larger mean value when compared to the results obtained when such fluctuations are neglected. In terms of dielectric constants, the reconciliation between the greater mean dipole moment and experimental indications that the dielectric constant of H2O ice is lower than that of D2O ice would indicate that the topology of the HB network is sensitive to protonic quantum fluctuations.

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

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

NASA Astrophysics Data System (ADS)

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

2018-03-01

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

Transient chaos - a resolution of breakdown of quantum-classical correspondence in optomechanics.

PubMed

Wang, Guanglei; Lai, Ying-Cheng; Grebogi, Celso

2016-10-17

Recently, the phenomenon of quantum-classical correspondence breakdown was uncovered in optomechanics, where in the classical regime the system exhibits chaos but in the corresponding quantum regime the motion is regular - there appears to be no signature of classical chaos whatsoever in the corresponding quantum system, generating a paradox. We find that transient chaos, besides being a physically meaningful phenomenon by itself, provides a resolution. Using the method of quantum state diffusion to simulate the system dynamics subject to continuous homodyne detection, we uncover transient chaos associated with quantum trajectories. The transient behavior is consistent with chaos in the classical limit, while the long term evolution of the quantum system is regular. Transient chaos thus serves as a bridge for the quantum-classical transition (QCT). Strikingly, as the system transitions from the quantum to the classical regime, the average chaotic transient lifetime increases dramatically (faster than the Ehrenfest time characterizing the QCT for isolated quantum systems). We develop a physical theory to explain the scaling law.

Transient chaos - a resolution of breakdown of quantum-classical correspondence in optomechanics

PubMed Central

Wang, Guanglei; Lai, Ying-Cheng; Grebogi, Celso

2016-01-01

Recently, the phenomenon of quantum-classical correspondence breakdown was uncovered in optomechanics, where in the classical regime the system exhibits chaos but in the corresponding quantum regime the motion is regular - there appears to be no signature of classical chaos whatsoever in the corresponding quantum system, generating a paradox. We find that transient chaos, besides being a physically meaningful phenomenon by itself, provides a resolution. Using the method of quantum state diffusion to simulate the system dynamics subject to continuous homodyne detection, we uncover transient chaos associated with quantum trajectories. The transient behavior is consistent with chaos in the classical limit, while the long term evolution of the quantum system is regular. Transient chaos thus serves as a bridge for the quantum-classical transition (QCT). Strikingly, as the system transitions from the quantum to the classical regime, the average chaotic transient lifetime increases dramatically (faster than the Ehrenfest time characterizing the QCT for isolated quantum systems). We develop a physical theory to explain the scaling law. PMID:27748418

Four-electron model for singlet and triplet excitation energy transfers with inclusion of coherence memory, inelastic tunneling and nuclear quantum effects

NASA Astrophysics Data System (ADS)

Suzuki, Yosuke; Ebina, Kuniyoshi; Tanaka, Shigenori

2016-08-01

A computational scheme to describe the coherent dynamics of excitation energy transfer (EET) in molecular systems is proposed on the basis of generalized master equations with memory kernels. This formalism takes into account those physical effects in electron-bath coupling system such as the spin symmetry of excitons, the inelastic electron tunneling and the quantum features of nuclear motions, thus providing a theoretical framework to perform an ab initio description of EET through molecular simulations for evaluating the spectral density and the temporal correlation function of electronic coupling. Some test calculations have then been carried out to investigate the dependence of exciton population dynamics on coherence memory, inelastic tunneling correlation time, magnitude of electronic coupling, quantum correction to temporal correlation function, reorganization energy and energy gap.

Deterministic generation of remote entanglement with active quantum feedback

DOE PAGES

Martin, Leigh; Motzoi, Felix; Li, Hanhan; ...

2015-12-10

We develop and study protocols for deterministic remote entanglement generation using quantum feedback, without relying on an entangling Hamiltonian. In order to formulate the most effective experimentally feasible protocol, we introduce the notion of average-sense locally optimal feedback protocols, which do not require real-time quantum state estimation, a difficult component of real-time quantum feedback control. We use this notion of optimality to construct two protocols that can deterministically create maximal entanglement: a semiclassical feedback protocol for low-efficiency measurements and a quantum feedback protocol for high-efficiency measurements. The latter reduces to direct feedback in the continuous-time limit, whose dynamics can bemore » modeled by a Wiseman-Milburn feedback master equation, which yields an analytic solution in the limit of unit measurement efficiency. Our formalism can smoothly interpolate between continuous-time and discrete-time descriptions of feedback dynamics and we exploit this feature to derive a superior hybrid protocol for arbitrary nonunit measurement efficiency that switches between quantum and semiclassical protocols. Lastly, we show using simulations incorporating experimental imperfections that deterministic entanglement of remote superconducting qubits may be achieved with current technology using the continuous-time feedback protocol alone.« less

Emulating Many-Body Localization with a Superconducting Quantum Processor

NASA Astrophysics Data System (ADS)

Xu, Kai; Chen, Jin-Jun; Zeng, Yu; Zhang, Yu-Ran; Song, Chao; Liu, Wuxin; Guo, Qiujiang; Zhang, Pengfei; Xu, Da; Deng, Hui; Huang, Keqiang; Wang, H.; Zhu, Xiaobo; Zheng, Dongning; Fan, Heng

2018-02-01

The law of statistical physics dictates that generic closed quantum many-body systems initialized in nonequilibrium will thermalize under their own dynamics. However, the emergence of many-body localization (MBL) owing to the interplay between interaction and disorder, which is in stark contrast to Anderson localization, which only addresses noninteracting particles in the presence of disorder, greatly challenges this concept, because it prevents the systems from evolving to the ergodic thermalized state. One critical evidence of MBL is the long-time logarithmic growth of entanglement entropy, and a direct observation of it is still elusive due to the experimental challenges in multiqubit single-shot measurement and quantum state tomography. Here we present an experiment fully emulating the MBL dynamics with a 10-qubit superconducting quantum processor, which represents a spin-1 /2 X Y model featuring programmable disorder and long-range spin-spin interactions. We provide essential signatures of MBL, such as the imbalance due to the initial nonequilibrium, the violation of eigenstate thermalization hypothesis, and, more importantly, the direct evidence of the long-time logarithmic growth of entanglement entropy. Our results lay solid foundations for precisely simulating the intriguing physics of quantum many-body systems on the platform of large-scale multiqubit superconducting quantum processors.

Nuclear quantum effects on the structure and the dynamics of [H2O]8 at low temperatures.

PubMed

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

2013-11-07

We use ring-polymer-molecular-dynamics (RPMD) techniques and the semi-empirical q-TIP4P/F water model to investigate the relationship between hydrogen bond connectivity and the characteristics of nuclear position fluctuations, including explicit incorporation of quantum effects, for the energetically low lying isomers of the prototype cluster [H2O]8 at T = 50 K and at 150 K. Our results reveal that tunneling and zero-point energy effects lead to sensible increments in the magnitudes of the fluctuations of intra and intermolecular distances. The degree of proton spatial delocalization is found to map logically with the hydrogen-bond connectivity pattern of the cluster. Dangling hydrogen bonds exhibit the largest extent of spatial delocalization and participate in shorter intramolecular O-H bonds. Combined effects from quantum and polarization fluctuations on the resulting individual dipole moments are also examined. From the dynamical side, we analyze the characteristics of the infrared absorption spectrum. The incorporation of nuclear quantum fluctuations promotes red shifts and sensible broadening relative to the classical profile, bringing the simulation results in much more satisfactory agreement with direct experimental information in the mid and high frequency range of the stretching band. While RPMD predictions overestimate the peak position of the low frequency shoulder, the overall agreement with that reported using an accurate, parameterized, many-body potential is reasonable, and far superior to that one obtains by implementing a partially adiabatic centroid molecular dynamics approach. Quantum effects on the collective dynamics, as reported by instantaneous normal modes, are also discussed.

A Combined Theoretical and Experimental Study for Silver Electroplating

PubMed Central

Liu, Anmin; Ren, Xuefeng; An, Maozhong; Zhang, Jinqiu; Yang, Peixia; Wang, Bo; Zhu, Yongming; Wang, Chong

2014-01-01

A novel method combined theoretical and experimental study for environmental friendly silver electroplating was introduced. Quantum chemical calculations and molecular dynamic (MD) simulations were employed for predicting the behaviour and function of the complexing agents. Electronic properties, orbital information, and single point energies of the 5,5-dimethylhydantoin (DMH), nicotinic acid (NA), as well as their silver(I)-complexes were provided by quantum chemical calculations based on density functional theory (DFT). Adsorption behaviors of the agents on copper and silver surfaces were investigated using MD simulations. Basing on the data of quantum chemical calculations and MD simulations, we believed that DMH and NA could be the promising complexing agents for silver electroplating. The experimental results, including of electrochemical measurement and silver electroplating, further confirmed the above prediction. This efficient and versatile method thus opens a new window to study or design complexing agents for generalized metal electroplating and will vigorously promote the level of this research region. PMID:24452389

Controlled exciton transfer between quantum dots with acoustic phonons taken into account

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

Golovinski, P. A., E-mail: golovinski@bk.ru

2015-09-15

A system of excitons in two quantum dots coupled by the dipole–dipole interaction is investigated. The excitation transfer process controlled by the optical Stark effect at nonresonant frequencies is considered and the effect of the interaction between excitons and acoustic phonons in a medium on this process is taken into account. The system evolution is described using quantum Heisenberg equations. A truncated set of equations is obtained and the transfer dynamics is numerically simulated. High-efficiency picosecond switching of the excitation transfer by a laser pulse with a rectangular envelope is demonstrated. The dependence of picosecond switching on the quantum-dot parametersmore » and optical-pulse length is presented.« less

Fidelity for kicked atoms with gravity near a quantum resonance.

PubMed

Dubertrand, Rémy; Guarneri, Italo; Wimberger, Sandro

2012-03-01

Kicked atoms under a constant Stark or gravity field are investigated for experimental setups with cold and ultracold atoms. The parametric stability of the quantum dynamics is studied using the fidelity. In the case of a quantum resonance, it is shown that the behavior of the fidelity depends on arithmetic properties of the gravity parameter. Close to a quantum resonance, the long-time asymptotics of the fidelity is studied by means of a pseudoclassical approximation introduced by Fishman et al. [J. Stat. Phys. 110, 911 (2003)]. The long-time decay of fidelity arises from the tunneling out of pseudoclassical stable islands, and a simple ansatz is proposed which satisfactorily reproduces the main features observed in numerical simulations.

Discrete-Time Quantum Walk with Phase Disorder: Localization and Entanglement Entropy.

PubMed

Zeng, Meng; Yong, Ee Hou

2017-09-20

Quantum Walk (QW) has very different transport properties to its classical counterpart due to interference effects. Here we study the discrete-time quantum walk (DTQW) with on-site static/dynamic phase disorder following either binary or uniform distribution in both one and two dimensions. For one dimension, we consider the Hadamard coin; for two dimensions, we consider either a 2-level Hadamard coin (Hadamard walk) or a 4-level Grover coin (Grover walk) for the rotation in coin-space. We study the transport properties e.g. inverse participation ratio (IPR) and the standard deviation of the density function (σ) as well as the coin-position entanglement entropy (EE), due to the two types of phase disorders and the two types of coins. Our numerical simulations show that the dimensionality, the type of coins, and whether the disorder is static or dynamic play a pivotal role and lead to interesting behaviors of the DTQW. The distribution of the phase disorder has very minor effects on the quantum walk.

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

Path-integral molecular dynamics simulations of hydrated hydrogen chloride cluster HCl(H 2O) 4 on a semiempirical potential energy surface

NASA Astrophysics Data System (ADS)

Takayanagi, Toshiyuki; Takahashi, Kenta; Kakizaki, Akira; Shiga, Motoyuki; Tachikawa, Masanori

2009-04-01

Path-integral molecular dynamics simulations for the HCl(H 2O) 4 cluster have been performed on the ground-state potential energy surface directly obtained on-the-fly from semiempirical PM3-MAIS molecular orbital calculations. It is found that the HCl(H 2O) 4 cluster has structural rearrangement above the temperature of 300 K showing a liquid-like behavior. Quantum mechanical fluctuation of hydrogen nuclei plays a significant role in structural arrangement processes in this cluster.

Computer Series, 29: Bits and Pieces, 10.

ERIC Educational Resources Information Center

Moore, John W., Ed.

1982-01-01

Describes computer programs (available from authors) including molecular input to computer, programs for quantum chemistry, library orientation to technical literature, plotting potentiometric titration data, simulating oscilloscope curves, organic qualitative analysis with dynamic graphics, extended Huckel calculations, and calculator programs…

Stochastic solution to quantum dynamics

NASA Technical Reports Server (NTRS)

John, Sarah; Wilson, John W.

1994-01-01

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

A Comparative Study of [CaEDTA](2-) and [MgEDTA](2-): Structural and Dynamical Insights from Quantum Mechanical Charge Field Molecular Dynamics.

PubMed

Tirler, Andreas O; Hofer, Thomas S

2015-07-09

Structure and dynamics of [MgEDTA](2-) and [CaEDTA](2-) complexes in aqueous solution have been investigated via quantum mechanical/molecular mechanical (QM/MM) simulations. While for the first a 6-fold octahedral complex has been observed, the presence of an additional coordinating water ligand has been observed in the latter case. Because of rapidly exchanging water molecules, this 7-fold coordination complex was found to form pentagonal bipyramidal as well as capped trigonal prismatic configurations along the simulation interchanging on the picosecond time scale. Also in the case of [MgEDTA](2-) a trigonal prismatic configuration has been observed for a very short time period of approximately 1 ps. This work reports for the first time the presence of trigonal prismatic structures observed in the coordination sphere of [MgEDTA](2-) and [CaEDTA](2-) complexes in aqueous solution. In addition to the detailed characterization of structure and dynamics of the systems, the prediction of the associated infrared spectra indicates that the ion-water vibrational mode found at approximately 250 cm(-1) provides a distinctive measure to experimentally detect the presence of the coordinating water molecule via low-frequency IR setups.

Approximate Quantum Dynamics using Ab Initio Classical Separable Potentials: Spectroscopic Applications.

PubMed

Hirshberg, Barak; Sagiv, Lior; Gerber, R Benny

2017-03-14

Algorithms for quantum molecular dynamics simulations that directly use ab initio methods have many potential applications. In this article, the ab initio classical separable potentials (AICSP) method is proposed as the basis for approximate algorithms of this type. The AICSP method assumes separability of the total time-dependent wave function of the nuclei and employs mean-field potentials that govern the dynamics of each degree of freedom. In the proposed approach, the mean-field potentials are determined by classical ab initio molecular dynamics simulations. The nuclear wave function can thus be propagated in time using the effective potentials generated "on the fly". As a test of the method for realistic systems, calculations of the stationary anharmonic frequencies of hydrogen stretching modes were carried out for several polyatomic systems, including three amino acids and the guanine-cytosine pair of nucleobases. Good agreement with experiments was found. The method scales very favorably with the number of vibrational modes and should be applicable for very large molecules, e.g., peptides. The method should also be applicable for properties such as vibrational line widths and line shapes. Work in these directions is underway.

Computation of Molecular Spectra on a Quantum Processor with an Error-Resilient Algorithm

DOE PAGES

Colless, J. I.; Ramasesh, V. V.; Dahlen, D.; ...

2018-02-12

Harnessing the full power of nascent quantum processors requires the efficient management of a limited number of quantum bits with finite coherent lifetimes. Hybrid algorithms, such as the variational quantum eigensolver (VQE), leverage classical resources to reduce the required number of quantum gates. Experimental demonstrations of VQE have resulted in calculation of Hamiltonian ground states, and a new theoretical approach based on a quantum subspace expansion (QSE) has outlined a procedure for determining excited states that are central to dynamical processes. Here, we use a superconducting-qubit-based processor to apply the QSE approach to the H 2 molecule, extracting both groundmore » and excited states without the need for auxiliary qubits or additional minimization. Further, we show that this extended protocol can mitigate the effects of incoherent errors, potentially enabling larger-scale quantum simulations without the need for complex error-correction techniques.« less

Computation of Molecular Spectra on a Quantum Processor with an Error-Resilient Algorithm

NASA Astrophysics Data System (ADS)

Colless, J. I.; Ramasesh, V. V.; Dahlen, D.; Blok, M. S.; Kimchi-Schwartz, M. E.; McClean, J. R.; Carter, J.; de Jong, W. A.; Siddiqi, I.

2018-02-01

Harnessing the full power of nascent quantum processors requires the efficient management of a limited number of quantum bits with finite coherent lifetimes. Hybrid algorithms, such as the variational quantum eigensolver (VQE), leverage classical resources to reduce the required number of quantum gates. Experimental demonstrations of VQE have resulted in calculation of Hamiltonian ground states, and a new theoretical approach based on a quantum subspace expansion (QSE) has outlined a procedure for determining excited states that are central to dynamical processes. We use a superconducting-qubit-based processor to apply the QSE approach to the H2 molecule, extracting both ground and excited states without the need for auxiliary qubits or additional minimization. Further, we show that this extended protocol can mitigate the effects of incoherent errors, potentially enabling larger-scale quantum simulations without the need for complex error-correction techniques.

Computation of Molecular Spectra on a Quantum Processor with an Error-Resilient Algorithm

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

Colless, J. I.; Ramasesh, V. V.; Dahlen, D.

Harnessing the full power of nascent quantum processors requires the efficient management of a limited number of quantum bits with finite coherent lifetimes. Hybrid algorithms, such as the variational quantum eigensolver (VQE), leverage classical resources to reduce the required number of quantum gates. Experimental demonstrations of VQE have resulted in calculation of Hamiltonian ground states, and a new theoretical approach based on a quantum subspace expansion (QSE) has outlined a procedure for determining excited states that are central to dynamical processes. Here, we use a superconducting-qubit-based processor to apply the QSE approach to the H 2 molecule, extracting both groundmore » and excited states without the need for auxiliary qubits or additional minimization. Further, we show that this extended protocol can mitigate the effects of incoherent errors, potentially enabling larger-scale quantum simulations without the need for complex error-correction techniques.« less

From transistor to trapped-ion computers for quantum chemistry.

PubMed

Yung, M-H; Casanova, J; Mezzacapo, A; McClean, J; Lamata, L; Aspuru-Guzik, A; Solano, E

2014-01-07

Over the last few decades, quantum chemistry has progressed through the development of computational methods based on modern digital computers. However, these methods can hardly fulfill the exponentially-growing resource requirements when applied to large quantum systems. As pointed out by Feynman, this restriction is intrinsic to all computational models based on classical physics. Recently, the rapid advancement of trapped-ion technologies has opened new possibilities for quantum control and quantum simulations. Here, we present an efficient toolkit that exploits both the internal and motional degrees of freedom of trapped ions for solving problems in quantum chemistry, including molecular electronic structure, molecular dynamics, and vibronic coupling. We focus on applications that go beyond the capacity of classical computers, but may be realizable on state-of-the-art trapped-ion systems. These results allow us to envision a new paradigm of quantum chemistry that shifts from the current transistor to a near-future trapped-ion-based technology.

From transistor to trapped-ion computers for quantum chemistry

PubMed Central

Yung, M.-H.; Casanova, J.; Mezzacapo, A.; McClean, J.; Lamata, L.; Aspuru-Guzik, A.; Solano, E.

2014-01-01

Over the last few decades, quantum chemistry has progressed through the development of computational methods based on modern digital computers. However, these methods can hardly fulfill the exponentially-growing resource requirements when applied to large quantum systems. As pointed out by Feynman, this restriction is intrinsic to all computational models based on classical physics. Recently, the rapid advancement of trapped-ion technologies has opened new possibilities for quantum control and quantum simulations. Here, we present an efficient toolkit that exploits both the internal and motional degrees of freedom of trapped ions for solving problems in quantum chemistry, including molecular electronic structure, molecular dynamics, and vibronic coupling. We focus on applications that go beyond the capacity of classical computers, but may be realizable on state-of-the-art trapped-ion systems. These results allow us to envision a new paradigm of quantum chemistry that shifts from the current transistor to a near-future trapped-ion-based technology. PMID:24395054

Single atom array to form a Rydberg ring

NASA Astrophysics Data System (ADS)

Zhan, Mingsheng; Xu, Peng; He, Xiaodong; Liu, Min; Wang, Jin

2012-02-01

Single atom arrays are ideal quantum systems for studying few-body quantum simulation and quantum computation [1]. Towards realizing a fully controllable array we did a lot of experimental efforts, which include rotating single atoms in a ring optical lattice generated by a spatial light modulator [2], high efficient loading of two atoms into a microscopic optical trap by dynamically reshaping the trap with a spatial light modulator [3], and trapping a single atom in a blue detuned optical bottle beam trap [4]. Recently, we succeeded in trapping up to 6 atoms in a ring optical lattice with one atom in each site. Further laser cooling the array and manipulation of the inner states will provide chance to form Ryberg rings for quantum simulation. [4pt] [1] M. Saffman et al., Rev. Mod. Phys. 82, 2313 (2010)[0pt] [2] X.D. He et al., Opt. Express 17, 21014 (2009)[0pt] [3] X.D. He et al., Opt. Express 18, 13586 (2010)[0pt] [4] P. Xu et al., Opt. Lett. 35, 2164 (2010)

A divide-conquer-recombine algorithmic paradigm for large spatiotemporal quantum molecular dynamics simulations

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

Shimojo, Fuyuki; Hattori, Shinnosuke; Department of Physics, Kumamoto University, Kumamoto 860-8555

We introduce an extension of the divide-and-conquer (DC) algorithmic paradigm called divide-conquer-recombine (DCR) to perform large quantum molecular dynamics (QMD) simulations on massively parallel supercomputers, in which interatomic forces are computed quantum mechanically in the framework of density functional theory (DFT). In DCR, the DC phase constructs globally informed, overlapping local-domain solutions, which in the recombine phase are synthesized into a global solution encompassing large spatiotemporal scales. For the DC phase, we design a lean divide-and-conquer (LDC) DFT algorithm, which significantly reduces the prefactor of the O(N) computational cost for N electrons by applying a density-adaptive boundary condition at themore » peripheries of the DC domains. Our globally scalable and locally efficient solver is based on a hybrid real-reciprocal space approach that combines: (1) a highly scalable real-space multigrid to represent the global charge density; and (2) a numerically efficient plane-wave basis for local electronic wave functions and charge density within each domain. Hybrid space-band decomposition is used to implement the LDC-DFT algorithm on parallel computers. A benchmark test on an IBM Blue Gene/Q computer exhibits an isogranular parallel efficiency of 0.984 on 786 432 cores for a 50.3 × 10{sup 6}-atom SiC system. As a test of production runs, LDC-DFT-based QMD simulation involving 16 661 atoms is performed on the Blue Gene/Q to study on-demand production of hydrogen gas from water using LiAl alloy particles. As an example of the recombine phase, LDC-DFT electronic structures are used as a basis set to describe global photoexcitation dynamics with nonadiabatic QMD (NAQMD) and kinetic Monte Carlo (KMC) methods. The NAQMD simulations are based on the linear response time-dependent density functional theory to describe electronic excited states and a surface-hopping approach to describe transitions between the excited states. A series of techniques are employed for efficiently calculating the long-range exact exchange correction and excited-state forces. The NAQMD trajectories are analyzed to extract the rates of various excitonic processes, which are then used in KMC simulation to study the dynamics of the global exciton flow network. This has allowed the study of large-scale photoexcitation dynamics in 6400-atom amorphous molecular solid, reaching the experimental time scales.« less

Development of reactive force fields using ab initio molecular dynamics simulation minimally biased to experimental data

NASA Astrophysics Data System (ADS)

Chen, Chen; Arntsen, Christopher; Voth, Gregory A.

2017-10-01

Incorporation of quantum mechanical electronic structure data is necessary to properly capture the physics of many chemical processes. Proton hopping in water, which involves rearrangement of chemical and hydrogen bonds, is one such example of an inherently quantum mechanical process. Standard ab initio molecular dynamics (AIMD) methods, however, do not yet accurately predict the structure of water and are therefore less than optimal for developing force fields. We have instead utilized a recently developed method which minimally biases AIMD simulations to match limited experimental data to develop novel multiscale reactive molecular dynamics (MS-RMD) force fields by using relative entropy minimization. In this paper, we present two new MS-RMD models using such a parameterization: one which employs water with harmonic internal vibrations and another which uses anharmonic water. We show that the newly developed MS-RMD models very closely reproduce the solvation structure of the hydrated excess proton in the target AIMD data. We also find that the use of anharmonic water increases proton hopping, thereby increasing the proton diffusion constant.

Structure of cold nuclear matter at subnuclear densities by quantum molecular dynamics

NASA Astrophysics Data System (ADS)

Watanabe, Gentaro; Sato, Katsuhiko; Yasuoka, Kenji; Ebisuzaki, Toshikazu

2003-09-01

Structure of cold nuclear matter at subnuclear densities for the proton fraction x=0.5, 0.3, and 0.1 is investigated by quantum molecular dynamics (QMD) simulations. We demonstrate that the phases with slablike and rodlike nuclei, etc. can be formed dynamically from hot uniform nuclear matter without any assumptions on nuclear shape, and also systematically analyze the structure of cold matter using two-point correlation functions and Minkowski functionals. In our simulations, we also observe intermediate phases, which have complicated nuclear shapes. It has been found out that these phases can be characterized as those with negative Euler characteristic. Our result implies the existence of these kinds of phases in addition to the simple “pasta” phases in neutron star crusts and supernova inner cores. In addition, we investigate the properties of the effective QMD interaction used in the present work to examine the validity of our results. The resultant energy per nucleon ɛn of the pure neutron matter, the proton chemical μ(0)p in pure neutron matter and the nuclear surface tension Esurf are generally reasonable in comparison with other nuclear interactions.

Mixed quantum-classical electrodynamics: Understanding spontaneous decay and zero-point energy

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

Li, Tao E.; Nitzan, Abraham; Sukharev, Maxim

The dynamics of an electronic two-level system coupled to an electromagnetic field are simulated explicitly for one- and three-dimensional systems through semiclassical propagation of the Maxwell-Liouville equations. Here, we consider three flavors of mixed quantum-classical dynamics: (i) the classical path approximation (CPA), (ii) Ehrenfest dynamics, and (iii) symmetrical quasiclassical (SQC) dynamics. Our findings are as follows: (i) The CPA fails to recover a consistent description of spontaneous emission, (ii) a consistent “spontaneous” emission can be obtained from Ehrenfest dynamics, provided that one starts in an electronic superposition state, and (iii) spontaneous emission is always obtained using SQC dynamics. Using themore » SQC and Ehrenfest frameworks, we further calculate the dynamics following an incoming pulse, but here we find very different responses: SQC and Ehrenfest dynamics deviate sometimes strongly in the calculated rate of decay of the transient excited state. Nevertheless, our work confirms the earlier observations by Miller [J. Chem. Phys. 69, 2188 (1978)] that Ehrenfest dynamics can effectively describe some aspects of spontaneous emission and highlights interesting possibilities for studying light-matter interactions with semiclassical mechanics.« less

Mixed quantum-classical electrodynamics: Understanding spontaneous decay and zero-point energy

NASA Astrophysics Data System (ADS)

Li, Tao E.; Nitzan, Abraham; Sukharev, Maxim; Martinez, Todd; Chen, Hsing-Ta; Subotnik, Joseph E.

2018-03-01

The dynamics of an electronic two-level system coupled to an electromagnetic field are simulated explicitly for one- and three-dimensional systems through semiclassical propagation of the Maxwell-Liouville equations. We consider three flavors of mixed quantum-classical dynamics: (i) the classical path approximation (CPA), (ii) Ehrenfest dynamics, and (iii) symmetrical quasiclassical (SQC) dynamics. Our findings are as follows: (i) The CPA fails to recover a consistent description of spontaneous emission, (ii) a consistent "spontaneous" emission can be obtained from Ehrenfest dynamics, provided that one starts in an electronic superposition state, and (iii) spontaneous emission is always obtained using SQC dynamics. Using the SQC and Ehrenfest frameworks, we further calculate the dynamics following an incoming pulse, but here we find very different responses: SQC and Ehrenfest dynamics deviate sometimes strongly in the calculated rate of decay of the transient excited state. Nevertheless, our work confirms the earlier observations by Miller [J. Chem. Phys. 69, 2188 (1978), 10.1063/1.436793] that Ehrenfest dynamics can effectively describe some aspects of spontaneous emission and highlights interesting possibilities for studying light-matter interactions with semiclassical mechanics.

Mixed quantum-classical electrodynamics: Understanding spontaneous decay and zero-point energy

DOE PAGES

Li, Tao E.; Nitzan, Abraham; Sukharev, Maxim; ...

2018-03-12

The dynamics of an electronic two-level system coupled to an electromagnetic field are simulated explicitly for one- and three-dimensional systems through semiclassical propagation of the Maxwell-Liouville equations. Here, we consider three flavors of mixed quantum-classical dynamics: (i) the classical path approximation (CPA), (ii) Ehrenfest dynamics, and (iii) symmetrical quasiclassical (SQC) dynamics. Our findings are as follows: (i) The CPA fails to recover a consistent description of spontaneous emission, (ii) a consistent “spontaneous” emission can be obtained from Ehrenfest dynamics, provided that one starts in an electronic superposition state, and (iii) spontaneous emission is always obtained using SQC dynamics. Using themore » SQC and Ehrenfest frameworks, we further calculate the dynamics following an incoming pulse, but here we find very different responses: SQC and Ehrenfest dynamics deviate sometimes strongly in the calculated rate of decay of the transient excited state. Nevertheless, our work confirms the earlier observations by Miller [J. Chem. Phys. 69, 2188 (1978)] that Ehrenfest dynamics can effectively describe some aspects of spontaneous emission and highlights interesting possibilities for studying light-matter interactions with semiclassical mechanics.« less

A path integral molecular dynamics study of the hyperfine coupling constants of the muoniated and hydrogenated acetone radicals

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

Oba, Yuki; Kawatsu, Tsutomu; Tachikawa, Masanori, E-mail: tachi@yokohama-cu.ac.jp

2016-08-14

The on-the-fly ab initio density functional path integral molecular dynamics (PIMD) simulations, which can account for both the nuclear quantum effect and thermal effect, were carried out to evaluate the structures and “reduced” isotropic hyperfine coupling constants (HFCCs) for muoniated and hydrogenated acetone radicals (2-muoxy-2-propyl and 2-hydoxy-2-propyl) in vacuo. The reduced HFCC value from a simple geometry optimization calculation without both the nuclear quantum effect and thermal effect is −8.18 MHz, and that by standard ab initio molecular dynamics simulation with only the thermal effect and without the nuclear quantum effect is 0.33 MHz at 300 K, where these twomore » methods cannot distinguish the difference between muoniated and hydrogenated acetone radicals. In contrast, the reduced HFCC value of the muoniated acetone radical by our PIMD simulation is 32.1 MHz, which is about 8 times larger than that for the hydrogenated radical of 3.97 MHz with the same level of calculation. We have found that the HFCC values are highly correlated with the local molecular structures; especially, the Mu—O bond length in the muoniated acetone radical is elongated due to the large nuclear quantum effect of the muon, which makes the expectation value of the HFCC larger. Although our PIMD result calculated in vacuo is about 4 times larger than the measured experimental value in aqueous solvent, the ratio of these HFCC values between muoniated and hydrogenated acetone radicals in vacuo is in reasonable agreement with the ratio of the experimental values in aqueous solvent (8.56 MHz and 0.9 MHz); the explicit presence of solvent molecules has a major effect on decreasing the reduced muon HFCC of in vacuo calculations for the quantitative reproduction.« less

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

NASA Astrophysics Data System (ADS)

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

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

Understanding the dielectric properties of water

NASA Astrophysics Data System (ADS)

Elton, Daniel Christopher

Liquid water is a complex material with many anomalous properties. Three of these anomalies are an abnormally high dielectric constant, an abnormally high boiling point, and a solid phase which is less dense than the liquid phase. Each of these anomalies is known to have been critically important in the development of life on Earth. All of water's special properties can be linked to water's unique ability to form hydrogen bonds. Water's hydrogen bonds form a transient network. Understanding the average structure of this network and how it changes through the phase diagram remains the focus of intense research. In this thesis we focus on understanding dielectric and infrared measurements, which measure the absorption and refraction of electromagnetic waves at different frequencies. Computer simulation is a necessary tool for correctly interpreting these measurements in terms of the microscopic dynamics of molecules. In the first part of this thesis we compare three classes of water molecule model that are used in molecular dynamics simulation--rigid, flexible, and polarizable. We show how the inclusion of polarization is necessary to capture how water's properties change with pressure and temperature. This finding is relevant to biophysical simulation. In the next part, we conduct a detailed study of water's dielectric properties to discover vibrational modes that propagate through the hydrogen bond network. Parts of the absorption spectrum of water are due to electromagnetic waves coupling to these modes. Previously, vibrational motions in water were thought to be confined to small clusters of perhaps five molecules. Our work upends this view by arguing that dynamics occur on the hydrogen bond network, resulting in modes that can propagate surprisingly long distances of up to two nanometers. These modes bear many similarities to optical phonon modes in ice. We show how the LO-TO splitting of these modes provides a new window into the structure of the hydrogen bond network. In the final part of this thesis we turn to the problems one encounters when trying to simulate water from "first principles'', ie. from the laws of quantum mechanics. The primary technique that physicists use to approximate the quantum mechanics of electrons, density functional theory, does not work well for water, and much work is being done to understand how to fix this problem. A usual assumption in first principles simulation is that only electrons need to be treated quantum mechanically. We argue that both electrons and nuclei need to be treated quantum mechanically and we present a new code to do this. The custom code presented in this thesis implements a novel algorithm which greatly speeds up the calculation of nuclear quantum effects with only minor losses in accuracy. We hope that others will start using our technique to advance first principles simulation. Accurate first principles simulation of water is important for understanding and developing solar water splitting catalysts and batteries. First principles simulations are also being increasingly used to understand proteins and drug molecules, and this trend will continue with Moore's law.

Experimental recovery of quantum correlations in absence of system-environment back-action

PubMed Central

Xu, Jin-Shi; Sun, Kai; Li, Chuan-Feng; Xu, Xiao-Ye; Guo, Guang-Can; Andersson, Erika; Lo Franco, Rosario; Compagno, Giuseppe

2013-01-01

Revivals of quantum correlations in composite open quantum systems are a useful dynamical feature against detrimental effects of the environment. Their occurrence is attributed to flows of quantum information back and forth from systems to quantum environments. However, revivals also show up in models where the environment is classical, thus unable to store quantum correlations, and forbids system-environment back-action. This phenomenon opens basic issues about its interpretation involving the role of classical environments, memory effects, collective effects and system-environment correlations. Moreover, an experimental realization of back-action-free quantum revivals has applicative relevance as it leads to recover quantum resources without resorting to more demanding structured environments and correction procedures. Here we introduce a simple two-qubit model suitable to address these issues. We then report an all-optical experiment which simulates the model and permits us to recover and control, against decoherence, quantum correlations without back-action. We finally give an interpretation of the phenomenon by establishing the roles of the involved parties. PMID:24287554

Experimental recovery of quantum correlations in absence of system-environment back-action.

PubMed

Xu, Jin-Shi; Sun, Kai; Li, Chuan-Feng; Xu, Xiao-Ye; Guo, Guang-Can; Andersson, Erika; Lo Franco, Rosario; Compagno, Giuseppe

2013-01-01

Revivals of quantum correlations in composite open quantum systems are a useful dynamical feature against detrimental effects of the environment. Their occurrence is attributed to flows of quantum information back and forth from systems to quantum environments. However, revivals also show up in models where the environment is classical, thus unable to store quantum correlations, and forbids system-environment back-action. This phenomenon opens basic issues about its interpretation involving the role of classical environments, memory effects, collective effects and system-environment correlations. Moreover, an experimental realization of back-action-free quantum revivals has applicative relevance as it leads to recover quantum resources without resorting to more demanding structured environments and correction procedures. Here we introduce a simple two-qubit model suitable to address these issues. We then report an all-optical experiment which simulates the model and permits us to recover and control, against decoherence, quantum correlations without back-action. We finally give an interpretation of the phenomenon by establishing the roles of the involved parties.

Improved real-time dynamics from imaginary frequency lattice simulations

NASA Astrophysics Data System (ADS)

Pawlowski, Jan M.; Rothkopf, Alexander

2018-03-01

The computation of real-time properties, such as transport coefficients or bound state spectra of strongly interacting quantum fields in thermal equilibrium is a pressing matter. Since the sign problem prevents a direct evaluation of these quantities, lattice data needs to be analytically continued from the Euclidean domain of the simulation to Minkowski time, in general an ill-posed inverse problem. Here we report on a novel approach to improve the determination of real-time information in the form of spectral functions by setting up a simulation prescription in imaginary frequencies. By carefully distinguishing between initial conditions and quantum dynamics one obtains access to correlation functions also outside the conventional Matsubara frequencies. In particular the range between ω0 and ω1 = 2πT, which is most relevant for the inverse problem may be more highly resolved. In combination with the fact that in imaginary frequencies the kernel of the inverse problem is not an exponential but only a rational function we observe significant improvements in the reconstruction of spectral functions, demonstrated in a simple 0+1 dimensional scalar field theory toy model.

Ultrafast hydrogen bond dynamics and partial electron transfer after photoexcitation of diethyl ester of 7-(diethylamino)-coumarin-3-phosphonic acid and its benzoxaphosphorin analog.

PubMed

Wagner, M S; Ilieva, E D; Petkov, P St; Nikolova, R D; Kienberger, R; Iglev, H

2015-04-21

The solvation dynamics after optical excitation of two phosphono-substituted coumarin derivatives dissolved in various solutions are studied by fluorescence up-conversion spectroscopy and quantum chemical simulations. The Kamlet-Taft analysis of the conventional absorption and emission spectra suggests weakening of the solvent-solute H-bonds upon optical excitation, which is in contrast to the results gained by the quantum simulations and earlier studies reported for coumarin derivatives without phosphono groups. The simulations give evidence that the solvent reorganisation around the excited fluorophore leads to partial electron transfer to the first solvation shell. The process occurs on a timescale between 1 and 10 ps depending on the solvent polarity and leads to a fast decay of the time-resolved emission signal. Using the ultrafast spectral shift of the time-dependent fluorescence we estimated the relaxation time of the H-bonds in the electronically excited state to be about 0.6 ps in water, 1.5 ps in ethanol and 2.8 ps in formamide.

Accuracy of buffered-force QM/MM simulations of silica

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

Peguiron, Anke; Moras, Gianpietro; Colombi Ciacchi, Lucio

2015-02-14

We report comparisons between energy-based quantum mechanics/molecular mechanics (QM/MM) and buffered force-based QM/MM simulations in silica. Local quantities—such as density of states, charges, forces, and geometries—calculated with both QM/MM approaches are compared to the results of full QM simulations. We find the length scale over which forces computed using a finite QM region converge to reference values obtained in full quantum-mechanical calculations is ∼10 Å rather than the ∼5 Å previously reported for covalent materials such as silicon. Electrostatic embedding of the QM region in the surrounding classical point charges gives only a minor contribution to the force convergence. Whilemore » the energy-based approach provides accurate results in geometry optimizations of point defects, we find that the removal of large force errors at the QM/MM boundary provided by the buffered force-based scheme is necessary for accurate constrained geometry optimizations where Si–O bonds are elongated and for finite-temperature molecular dynamics simulations of crack propagation. Moreover, the buffered approach allows for more flexibility, since special-purpose QM/MM coupling terms that link QM and MM atoms are not required and the region that is treated at the QM level can be adaptively redefined during the course of a dynamical simulation.« less

Structural, dynamic, and vibrational properties during heat transfer in Si/Ge superlattices: A Car-Parrinello molecular dynamics study

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

Ji, Pengfei; Zhang, Yuwen, E-mail: zhangyu@missouri.edu; Yang, Mo

The structural, dynamic, and vibrational properties during heat transfer process in Si/Ge superlattices are studied by analyzing the trajectories generated by the ab initio Car-Parrinello molecular dynamics simulation. The radial distribution functions and mean square displacements are calculated and further discussions are made to explain and probe the structural changes relating to the heat transfer phenomenon. Furthermore, the vibrational density of states of the two layers (Si/Ge) are computed and plotted to analyze the contributions of phonons with different frequencies to the heat conduction. Coherent heat conduction of the low frequency phonons is found and their contributions to facilitate heatmore » transfer are confirmed. The Car-Parrinello molecular dynamics simulation outputs in the work show reasonable thermophysical results of the thermal energy transport process and shed light on the potential applications of treating the heat transfer in the superlattices of semiconductor materials from a quantum mechanical molecular dynamics simulation perspective.« less

Structural, dynamic, and vibrational properties during heat transfer in Si/Ge superlattices: A Car-Parrinello molecular dynamics study

NASA Astrophysics Data System (ADS)

Ji, Pengfei; Zhang, Yuwen; Yang, Mo

2013-12-01

The structural, dynamic, and vibrational properties during heat transfer process in Si/Ge superlattices are studied by analyzing the trajectories generated by the ab initio Car-Parrinello molecular dynamics simulation. The radial distribution functions and mean square displacements are calculated and further discussions are made to explain and probe the structural changes relating to the heat transfer phenomenon. Furthermore, the vibrational density of states of the two layers (Si/Ge) are computed and plotted to analyze the contributions of phonons with different frequencies to the heat conduction. Coherent heat conduction of the low frequency phonons is found and their contributions to facilitate heat transfer are confirmed. The Car-Parrinello molecular dynamics simulation outputs in the work show reasonable thermophysical results of the thermal energy transport process and shed light on the potential applications of treating the heat transfer in the superlattices of semiconductor materials from a quantum mechanical molecular dynamics simulation perspective.

Electron-phonon interaction within classical molecular dynamics

DOE PAGES

Tamm, A.; Samolyuk, G.; Correa, A. A.; ...

2016-07-14

Here, we present a model for nonadiabatic classical molecular dynamics simulations that captures with high accuracy the wave-vector q dependence of the phonon lifetimes, in agreement with quantum mechanics calculations. It is based on a local view of the e-ph interaction where individual atom dynamics couples to electrons via a damping term that is obtained as the low-velocity limit of the stopping power of a moving ion in a host. The model is parameter free, as its components are derived from ab initio-type calculations, is readily extended to the case of alloys, and is adequate for large-scale molecular dynamics computermore » simulations. We also show how this model removes some oversimplifications of the traditional ionic damped dynamics commonly used to describe situations beyond the Born-Oppenheimer approximation.« less

Graph-based linear scaling electronic structure theory.

PubMed

Niklasson, Anders M N; Mniszewski, Susan M; Negre, Christian F A; Cawkwell, Marc J; Swart, Pieter J; Mohd-Yusof, Jamal; Germann, Timothy C; Wall, Michael E; Bock, Nicolas; Rubensson, Emanuel H; Djidjev, Hristo

2016-06-21

We show how graph theory can be combined with quantum theory to calculate the electronic structure of large complex systems. The graph formalism is general and applicable to a broad range of electronic structure methods and materials, including challenging systems such as biomolecules. The methodology combines well-controlled accuracy, low computational cost, and natural low-communication parallelism. This combination addresses substantial shortcomings of linear scaling electronic structure theory, in particular with respect to quantum-based molecular dynamics simulations.

Graph-based linear scaling electronic structure theory

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

Niklasson, Anders M. N., E-mail: amn@lanl.gov; Negre, Christian F. A.; Cawkwell, Marc J.

2016-06-21

We show how graph theory can be combined with quantum theory to calculate the electronic structure of large complex systems. The graph formalism is general and applicable to a broad range of electronic structure methods and materials, including challenging systems such as biomolecules. The methodology combines well-controlled accuracy, low computational cost, and natural low-communication parallelism. This combination addresses substantial shortcomings of linear scaling electronic structure theory, in particular with respect to quantum-based molecular dynamics simulations.

Abstractive dissociation of oxygen over Al(111): a nonadiabatic quantum model.

PubMed

Katz, Gil; Kosloff, Ronnie; Zeiri, Yehuda

2004-02-22

The dissociation of oxygen on a clean aluminum surface is studied theoretically. A nonadiabatic quantum dynamical model is used, based on four electronically distinct potential energy surfaces characterized by the extent of charge transfer from the metal to the adsorbate. A flat surface approximation is used to reduce the computation complexity. The conservation of the helicopter angular momentum allows Boltzmann averaging of the outcome of the propagation of a three degrees of freedom wave function. The dissociation event is simulated by solving the time-dependent Schrödinger equation for a period of 30 femtoseconds. As a function of incident kinetic energy, the dissociation yield follows the experimental trend. An attempt at simulation employing only the lowest adiabatic surface failed, qualitatively disagreeing with both experiment and nonadiabatic calculations. The final products, adsorptive dissociation and abstractive dissociation, are obtained by carrying out a semiclassical molecular dynamics simulation with surface hopping which describes the back charge transfer from an oxygen atom negative ion to the surface. The final adsorbed oxygen pair distribution compares well with experiment. By running the dynamical events backward in time, a correlation is established between the products and the initial conditions which lead to their production. Qualitative agreement is thus obtained with recent experiments that show suppression of abstraction by rotational excitation. (c) 2004 American Institute of Physics.

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

Non-radiative relaxation dynamics of pyrrole following excitation in the range 249.5-200 nm

NASA Astrophysics Data System (ADS)

Kirkby, Oliver M.; Parkes, Michael A.; Neville, Simon P.; Worth, Graham A.; Fielding, Helen H.

2017-09-01

The non-radiative relaxation dynamics of pyrrole have been investigated using time-resolved photoelectron spectroscopy and quantum dynamics simulations. Following excitation of the A2 (11 πσ∗) state, we observe population flow out of the Franck-Condon region on a ≲ 50 fs timescale. Following excitation of the B2 (21 ππ∗) state, we observe population being transferred to the A2 (11 πσ∗) state on a <50 fs timescale and subsequently out of the Franck-Condon region, also on a <50 fs timescale. Quantum dynamics calculations suggest that population is transferred from the B2 (21 ππ∗) state through the A2 (1 π 3pz) state to the B1 (21 πσ∗) state before being transferred to the A2 (11 πσ∗) state.

Magnetic field fluctuations analysis for the ion trap implementation of the quantum Rabi model in the deep strong coupling regime

NASA Astrophysics Data System (ADS)

Puebla, Ricardo; Casanova, Jorge; Plenio, Martin B.

2018-03-01

The dynamics of the quantum Rabi model (QRM) in the deep strong coupling regime is theoretically analyzed in a trapped-ion set-up. Recognizably, the main hallmark of this regime is the emergence of collapses and revivals, whose faithful observation is hindered under realistic magnetic dephasing noise. Here, we discuss how to attain a faithful implementation of the QRM in the deep strong coupling regime which is robust against magnetic field fluctuations and at the same time provides a large tunability of the simulated parameters. This is achieved by combining standing wave laser configuration with continuous dynamical decoupling. In addition, we study the role that amplitude fluctuations play to correctly attain the QRM using the proposed method. In this manner, the present work further supports the suitability of continuous dynamical decoupling techniques in trapped-ion settings to faithfully realize different interacting dynamics.

i-PI: A Python interface for ab initio path integral molecular dynamics simulations

NASA Astrophysics Data System (ADS)

Ceriotti, Michele; More, Joshua; Manolopoulos, David E.

2014-03-01

Recent developments in path integral methodology have significantly reduced the computational expense of including quantum mechanical effects in the nuclear motion in ab initio molecular dynamics simulations. However, the implementation of these developments requires a considerable programming effort, which has hindered their adoption. Here we describe i-PI, an interface written in Python that has been designed to minimise the effort required to bring state-of-the-art path integral techniques to an electronic structure program. While it is best suited to first principles calculations and path integral molecular dynamics, i-PI can also be used to perform classical molecular dynamics simulations, and can just as easily be interfaced with an empirical forcefield code. To give just one example of the many potential applications of the interface, we use it in conjunction with the CP2K electronic structure package to showcase the importance of nuclear quantum effects in high-pressure water. Catalogue identifier: AERN_v1_0 Program summary URL: http://cpc.cs.qub.ac.uk/summaries/AERN_v1_0.html Program obtainable from: CPC Program Library, Queen’s University, Belfast, N. Ireland Licensing provisions: GNU General Public License, version 3 No. of lines in distributed program, including test data, etc.: 138626 No. of bytes in distributed program, including test data, etc.: 3128618 Distribution format: tar.gz Programming language: Python. Computer: Multiple architectures. Operating system: Linux, Mac OSX, Windows. RAM: Less than 256 Mb Classification: 7.7. External routines: NumPy Nature of problem: Bringing the latest developments in the modelling of nuclear quantum effects with path integral molecular dynamics to ab initio electronic structure programs with minimal implementational effort. Solution method: State-of-the-art path integral molecular dynamics techniques are implemented in a Python interface. Any electronic structure code can be patched to receive the atomic coordinates from the Python interface, and to return the forces and energy that are used to integrate the equations of motion. Restrictions: This code only deals with distinguishable particles. It does not include fermonic or bosonic exchanges between equivalent nuclei, which can become important at very low temperatures. Running time: Depends dramatically on the nature of the simulation being performed. A few minutes for short tests with empirical force fields, up to several weeks for production calculations with ab initio forces. The examples provided with the code run in less than an hour.

Structure and dynamics of the CrIII ion in aqueous solution: Ab initio QM/MM molecular dynamics simulation.

PubMed

Kritayakornupong, Chinapong; Plankensteiner, Kristof; Rode, Bernd M

2004-10-01

Structural and dynamical properties of the Cr(III) ion in aqueous solution have been investigated using a combined ab initio quantum mechanical/molecular mechanical (QM/MM) molecular dynamics simulation. The hydration structure of Cr(III) was determined in terms of radial distribution functions, coordination numbers, and angular distributions. The QM/MM simulation gives coordination numbers of 6 and 15.4 for the first and second hydration shell, respectively. The first hydration shell is kinetically very inert but by no means rigid and variations of the first hydration shell geometry lead to distinct splitting in the vibrational spectra of Cr(H(2)O)(6) (3+). A mean residence time of 22 ps was obtained for water ligands residing in the second hydration shell, which is remarkably shorter than the experimentally estimated value. The hydration energy of -1108 +/- 7 kcal/mol, obtained from the QM/MM simulation, corresponds well to the experimental hydration enthalpy value. Copyright 2004 Wiley Periodicals, Inc.

Reaching multi-nanosecond timescales in combined QM/MM molecular dynamics simulations through parallel horsetail sampling.

PubMed

Martins-Costa, Marilia T C; Ruiz-López, Manuel F

2017-04-15

We report an enhanced sampling technique that allows to reach the multi-nanosecond timescale in quantum mechanics/molecular mechanics molecular dynamics simulations. The proposed technique, called horsetail sampling, is a specific type of multiple molecular dynamics approach exhibiting high parallel efficiency. It couples a main simulation with a large number of shorter trajectories launched on independent processors at periodic time intervals. The technique is applied to study hydrogen peroxide at the water liquid-vapor interface, a system of considerable atmospheric relevance. A total simulation time of a little more than 6 ns has been attained for a total CPU time of 5.1 years representing only about 20 days of wall-clock time. The discussion of the results highlights the strong influence of the solvation effects at the interface on the structure and the electronic properties of the solute. © 2017 Wiley Periodicals, Inc. © 2017 Wiley Periodicals, Inc.

Semiclassical modelling of finite-pulse effects on non-adiabatic photodynamics via initial condition filtering: The predissociation of NaI as a test case

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

Martínez-Mesa, Aliezer; Institut für Chemie, Universität Potsdam, Karl-Liebknecht-Strasse 24-25, D-14476 Potsdam-Golm; Saalfrank, Peter

2015-05-21

Femtosecond-laser pulse driven non-adiabatic spectroscopy and dynamics in molecular and condensed phase systems continue to be a challenge for theoretical modelling. One of the main obstacles is the “curse of dimensionality” encountered in non-adiabatic, exact wavepacket propagation. A possible route towards treating complex molecular systems is via semiclassical surface-hopping schemes, in particular if they account not only for non-adiabatic post-excitation dynamics but also for the initial optical excitation. One such approach, based on initial condition filtering, will be put forward in what follows. As a simple test case which can be compared with exact wavepacket dynamics, we investigate the influencemore » of the different parameters determining the shape of a laser pulse (e.g., its finite width and a possible chirp) on the predissociation dynamics of a NaI molecule, upon photoexcitation of the A(0{sup +}) state. The finite-pulse effects are mapped into the initial conditions for semiclassical surface-hopping simulations. The simulated surface-hopping diabatic populations are in qualitative agreement with the quantum mechanical results, especially concerning the subpicosend photoinduced dynamics, the main deviations being the relative delay of the non-adiabatic transitions in the semiclassical picture. Likewise, these differences in the time-dependent electronic populations calculated via the semiclassical and the quantum methods are found to have a mild influence on the overall probability density distribution. As a result, the branching ratios between the bound and the dissociative reaction channels and the time-evolution of the molecular wavepacket predicted by the semiclassical method agree with those computed using quantum wavepacket propagation. Implications for more challenging molecular systems are given.« less

Realistic finite temperature simulations of magnetic systems using quantum statistics

NASA Astrophysics Data System (ADS)

Bergqvist, Lars; Bergman, Anders

2018-01-01

We have performed realistic atomistic simulations at finite temperatures using Monte Carlo and atomistic spin dynamics simulations incorporating quantum (Bose-Einstein) statistics. The description is much improved at low temperatures compared to classical (Boltzmann) statistics normally used in these kind of simulations, while at higher temperatures the classical statistics are recovered. This corrected low-temperature description is reflected in both magnetization and the magnetic specific heat, the latter allowing for improved modeling of the magnetic contribution to free energies. A central property in the method is the magnon density of states at finite temperatures, and we have compared several different implementations for obtaining it. The method has no restrictions regarding chemical and magnetic order of the considered materials. This is demonstrated by applying the method to elemental ferromagnetic systems, including Fe and Ni, as well as Fe-Co random alloys and the ferrimagnetic system GdFe3.

High-density amorphous ice: A path-integral simulation

NASA Astrophysics Data System (ADS)

Herrero, Carlos P.; Ramírez, Rafael

2012-09-01

Structural and thermodynamic properties of high-density amorphous (HDA) ice have been studied by path-integral molecular dynamics simulations in the isothermal-isobaric ensemble. Interatomic interactions were modeled by using the effective q-TIP4P/F potential for flexible water. Quantum nuclear motion is found to affect several observable properties of the amorphous solid. At low temperature (T = 50 K) the molar volume of HDA ice is found to increase by 6%, and the intramolecular O-H distance rises by 1.4% due to quantum motion. Peaks in the radial distribution function of HDA ice are broadened with respect to their classical expectancy. The bulk modulus, B, is found to rise linearly with the pressure, with a slope ∂B/∂P = 7.1. Our results are compared with those derived earlier from classical and path-integral simulations of HDA ice. We discuss similarities and discrepancies with those earlier simulations.

Many-body formulation of carriers capture time in quantum dots applicable in device simulation codes

NASA Astrophysics Data System (ADS)

Vallone, Marco

2010-03-01

We present an application of Green's functions formalism to calculate in a simplified but rigorous way electrons and holes capture time in quantum dots in closed form as function of carrier density, levels confinement potential, and temperature. Carrier-carrier (Auger) scattering and single LO-phonon emission are both addressed accounting for dynamic effects of the potential screening in the single plasmon pole approximation of the dielectric function. Regarding the LO-phonons interaction, the formulation evidences the role of the dynamic screening from wetting-layer carriers in comparison with its static limit, describes the interplay between screening and Fermi band filling, and offers simple expressions for capture time, suitable for modeling implementation.

Optical turbulence and transverse rogue waves in a cavity with triple-quantum-dot molecules

NASA Astrophysics Data System (ADS)

Eslami, M.; Khanmohammadi, M.; Kheradmand, R.; Oppo, G.-L.

2017-09-01

We show that optical turbulence extreme events can exist in the transverse dynamics of a cavity containing molecules of triple quantum dots under conditions close to tunneling-induced transparency. These nanostructures, when coupled via tunneling, form a four-level configuration with tunable energy-level separations. We show that such a system exhibits multistability and bistability of Turing structures in instability domains with different critical wave vectors. By numerical simulation of the mean-field equation that describes the transverse dynamics of the system, we show that the simultaneous presence of two transverse solutions with opposite nonlinearities gives rise to a series of turbulent structures with the capability of generating two-dimensional rogue waves.

Efficient analysis of mode profiles in elliptical microcavity using dynamic-thermal electron-quantum medium FDTD method.

PubMed

Khoo, E H; Ahmed, I; Goh, R S M; Lee, K H; Hung, T G G; Li, E P

2013-03-11

The dynamic-thermal electron-quantum medium finite-difference time-domain (DTEQM-FDTD) method is used for efficient analysis of mode profile in elliptical microcavity. The resonance peak of the elliptical microcavity is studied by varying the length ratio. It is observed that at some length ratios, cavity mode is excited instead of whispering gallery mode. This depicts that mode profiles are length ratio dependent. Through the implementation of the DTEQM-FDTD on graphic processing unit (GPU), the simulation time is reduced by 300 times as compared to the CPU. This leads to an efficient optimization approach to design microcavity lasers for wide range of applications in photonic integrated circuits.

Quantum dynamics of thermalizing systems

NASA Astrophysics Data System (ADS)

White, Christopher David; Zaletel, Michael; Mong, Roger S. K.; Refael, Gil

2018-01-01

We introduce a method "DMT" for approximating density operators of 1D systems that, when combined with a standard framework for time evolution (TEBD), makes possible simulation of the dynamics of strongly thermalizing systems to arbitrary times. We demonstrate that the method performs well for both near-equilibrium initial states (Gibbs states with spatially varying temperatures) and far-from-equilibrium initial states, including quenches across phase transitions and pure states.

Orbital effect of the magnetic field in dynamical mean-field theory

NASA Astrophysics Data System (ADS)

Acheche, S.; Arsenault, L.-F.; Tremblay, A.-M. S.

2017-12-01

The availability of large magnetic fields at international facilities and of simulated magnetic fields that can reach the flux-quantum-per-unit-area level in cold atoms calls for systematic studies of orbital effects of the magnetic field on the self-energy of interacting systems. Here we demonstrate theoretically that orbital effects of magnetic fields can be treated within single-site dynamical mean-field theory with a translationally invariant quantum impurity problem. As an example, we study the one-band Hubbard model on the square lattice using iterated perturbation theory as an impurity solver. We recover the expected quantum oscillations in the scattering rate, and we show that the magnetic fields allow the interaction-induced effective mass to be measured through the single-particle density of states accessible in tunneling experiments. The orbital effect of magnetic fields on scattering becomes particularly important in the Hofstadter butterfly regime.

Real-time monitoring of Lévy flights in a single quantum system

NASA Astrophysics Data System (ADS)

Issler, M.; Höller, J.; Imamoǧlu, A.

2016-02-01

Lévy flights are random walks where the dynamics is dominated by rare events. Even though they have been studied in vastly different physical systems, their observation in a single quantum system has remained elusive. Here we analyze a periodically driven open central spin system and demonstrate theoretically that the dynamics of the spin environment exhibits Lévy flights. For the particular realization in a single-electron charged quantum dot driven by periodic resonant laser pulses, we use Monte Carlo simulations to confirm that the long waiting times between successive nuclear spin-flip events are governed by a power-law distribution; the corresponding exponent η =-3 /2 can be directly measured in real time by observing the waiting time distribution of successive photon emission events. Remarkably, the dominant intrinsic limitation of the scheme arising from nuclear quadrupole coupling can be minimized by adjusting the magnetic field or by implementing spin echo.

Symmetrical Windowing for Quantum States in Quasi-Classical Trajectory Simulations

NASA Astrophysics Data System (ADS)

Cotton, Stephen Joshua

An approach has been developed for extracting approximate quantum state-to-state information from classical trajectory simulations which "quantizes" symmetrically both the initial and final classical actions associated with the degrees of freedom of interest using quantum number bins (or "window functions") which are significantly narrower than unit-width. This approach thus imposes a more stringent quantization condition on classical trajectory simulations than has been traditionally employed, while doing so in a manner that is time-symmetric and microscopically reversible. To demonstrate this "symmetric quasi-classical" (SQC) approach for a simple real system, collinear H + H2 reactive scattering calculations were performed [S.J. Cotton and W.H. Miller, J. Phys. Chem. A 117, 7190 (2013)] with SQC-quantization applied to the H 2 vibrational degree of freedom (DOF). It was seen that the use of window functions of approximately 1/2-unit width led to calculated reaction probabilities in very good agreement with quantum mechanical results over the threshold energy region, representing a significant improvement over what is obtained using the traditional quasi-classical procedure. The SQC approach was then applied [S.J. Cotton and W.H. Miller, J. Chem. Phys. 139, 234112 (2013)] to the much more interesting and challenging problem of incorporating non-adiabatic effects into what would otherwise be standard classical trajectory simulations. To do this, the classical Meyer-Miller (MM) Hamiltonian was used to model the electronic DOFs, with SQC-quantization applied to the classical "electronic" actions of the MM model---representing the occupations of the electronic states---in order to extract the electronic state population dynamics. It was demonstrated that if one ties the zero-point energy (ZPE) of the electronic DOFs to the SQC windowing function's width parameter this very simple SQC/MM approach is capable of quantitatively reproducing quantum mechanical results for a range of standard benchmark models of electronically non-adiabatic processes, including applications where "quantum" coherence effects are significant. Notably, among these benchmarks was the well-studied "spin-boson" model of condensed phase non-adiabatic dynamics, in both its symmetric and asymmetric forms---the latter of which many classical approaches fail to treat successfully. The SQC/MM approach to the treatment of non-adiabatic dynamics was next applied [S.J. Cotton, K. Igumenshchev, and W.H. Miller, J. Chem. Phys., 141, 084104 (2014)] to several recently proposed models of condensed phase electron transfer (ET) processes. For these problems, a flux-side correlation function framework modified for consistency with the SQC approach was developed for the calculation of thermal ET rate constants, and excellent accuracy was seen over wide ranges of non-adiabatic coupling strength and energetic bias/exothermicity. Significantly, the "inverted regime" in thermal rate constants (with increasing bias) known from Marcus Theory was reproduced quantitatively for these models---representing the successful treatment of another regime that classical approaches generally have difficulty in correctly describing. Relatedly, a model of photoinduced proton coupled electron transfer (PCET) was also addressed, and it was shown that the SQC/MM approach could reasonably model the explicit population dynamics of the photoexcited electron donor and acceptor states over the four parameter regimes considered. The potential utility of the SQC/MM technique lies in its stunning simplicity and the ease by which it may readily be incorporated into "ordinary" molecular dynamics (MD) simulations. In short, a typical MD simulation may be augmented to take non-adiabatic effects into account simply by introducing an auxiliary pair of classical "electronic" action-angle variables for each energetically viable Born-Oppenheimer surface, and time-evolving these auxiliary variables via Hamilton's equations (using the MM electronic Hamiltonian) in the same manner that the other classical variables---i.e., the coordinates of all the nuclei---are evolved forward in time. In a complex molecular system involving many hundreds or thousands of nuclear DOFs, the propagation of these extra "electronic" variables represents a modest increase in computational effort, and yet, the examples presented herein suggest that in many instances the SQC/MM approach will describe the true non-adiabatic quantum dynamics to a reasonable and useful degree of quantitative accuracy.

Enstrophy Cascade in Decaying Two-Dimensional Quantum Turbulence

NASA Astrophysics Data System (ADS)

Reeves, Matthew T.; Billam, Thomas P.; Yu, Xiaoquan; Bradley, Ashton S.

2017-11-01

We report evidence for an enstrophy cascade in large-scale point-vortex simulations of decaying two-dimensional quantum turbulence. Devising a method to generate quantum vortex configurations with kinetic energy narrowly localized near a single length scale, the dynamics are found to be well characterized by a superfluid Reynolds number Res that depends only on the number of vortices and the initial kinetic energy scale. Under free evolution the vortices exhibit features of a classical enstrophy cascade, including a k-3 power-law kinetic energy spectrum, and constant enstrophy flux associated with inertial transport to small scales. Clear signatures of the cascade emerge for N ≳500 vortices. Simulating up to very large Reynolds numbers (N =32 768 vortices), additional features of the classical theory are observed: the Kraichnan-Batchelor constant is found to converge to C'≈1.6 , and the width of the k-3 range scales as Res1 /2 .

Observing fermionic statistics with photons in arbitrary processes

PubMed Central

Matthews, Jonathan C. F.; Poulios, Konstantinos; Meinecke, Jasmin D. A.; Politi, Alberto; Peruzzo, Alberto; Ismail, Nur; Wörhoff, Kerstin; Thompson, Mark G.; O'Brien, Jeremy L.

2013-01-01

Quantum mechanics defines two classes of particles-bosons and fermions-whose exchange statistics fundamentally dictate quantum dynamics. Here we develop a scheme that uses entanglement to directly observe the correlated detection statistics of any number of fermions in any physical process. This approach relies on sending each of the entangled particles through identical copies of the process and by controlling a single phase parameter in the entangled state, the correlated detection statistics can be continuously tuned between bosonic and fermionic statistics. We implement this scheme via two entangled photons shared across the polarisation modes of a single photonic chip to directly mimic the fermion, boson and intermediate behaviour of two-particles undergoing a continuous time quantum walk. The ability to simulate fermions with photons is likely to have applications for verifying boson scattering and for observing particle correlations in analogue simulation using any physical platform that can prepare the entangled state prescribed here. PMID:23531788

The Quantum and Fluid Mechanics of Global Warming

NASA Astrophysics Data System (ADS)

Marston, Brad

2008-03-01

Quantum physics and fluid mechanics are the foundation of any understanding of the Earth's climate. In this talk I invoke three well-known aspects of quantum mechanics to explore what will happen as the concentrations of greenhouse gases such as carbon dioxide continue to increase. Fluid dynamical models of the Earth's atmosphere, demonstrated here in live simulations, yield further insight into past, present, and future climates. Statistics of geophysical flows can, however, be ascertained directly without recourse to numerical simulation, using concepts borrowed from nonequilibrium statistical mechanicsootnotetextJ. B. Marston, E. Conover, and Tapio Schneider, ``Statistics of an Unstable Barotropic Jet from a Cumulant Expansion,'' arXiv:0705.0011, J. Atmos. Sci. (in press).. I discuss several other ways that theoretical physics may be able to contribute to a deeper understanding of climate changeootnotetextJ. Carlson, J. Harte, G. Falkovich, J. B. Marston, and R. Pierrehumbert, ``Physics of Climate Change'' 2008 Program of the Kavli Institute for Theoretical Physics..

Satellite orbit determination using quantum correlation technology

NASA Astrophysics Data System (ADS)

Zhang, Bo; Sun, Fuping; Zhu, Xinhui; Jia, Xiaolin

2018-03-01

After the presentation of second-order correlation ranging principles with quantum entanglement, the concept of quantum measurement is introduced to dynamic satellite precise orbit determination. Based on the application of traditional orbit determination models for correcting the systematic errors within the satellite, corresponding models for quantum orbit determination (QOD) are established. This paper experiments on QOD with the BeiDou Navigation Satellite System (BDS) by first simulating quantum observations of 1 day arc-length. Then the satellite orbits are resolved and compared with the reference precise ephemerides. Subsequently, some related factors influencing the accuracy of QOD are discussed. Furthermore, the accuracy for GEO, IGSO and MEO satellites increase about 20, 30 and 10 times, respectively, compared with the results from the resolution by measured data. Therefore, it can be expected that quantum technology may also bring delightful surprises to satellite orbit determination as have already emerged in other fields.

Broadband multiresonator quantum memory-interface.

PubMed

Moiseev, S A; Gerasimov, K I; Latypov, R R; Perminov, N S; Petrovnin, K V; Sherstyukov, O N

2018-03-05

In this paper we experimentally demonstrated a broadband scheme of the multiresonator quantum memory-interface. The microwave photonic scheme consists of the system of mini-resonators strongly interacting with a common broadband resonator coupled with the external waveguide. We have implemented the impedance matched quantum storage in this scheme via controllable tuning of the mini-resonator frequencies and coupling of the common resonator with the external waveguide. Proof-of-principal experiment has been demonstrated for broadband microwave pulses when the quantum efficiency of 16.3% was achieved at room temperature. By using the obtained experimental spectroscopic data, the dynamics of the signal retrieval has been simulated and promising results were found for high-Q mini-resonators in microwave and optical frequency ranges. The results pave the way for the experimental implementation of broadband quantum memory-interface with quite high efficiency η > 0.99 on the basis of modern technologies, including optical quantum memory at room temperature.

Quantum-Inspired Multidirectional Associative Memory With a Self-Convergent Iterative Learning.

PubMed

Masuyama, Naoki; Loo, Chu Kiong; Seera, Manjeevan; Kubota, Naoyuki

2018-04-01

Quantum-inspired computing is an emerging research area, which has significantly improved the capabilities of conventional algorithms. In general, quantum-inspired hopfield associative memory (QHAM) has demonstrated quantum information processing in neural structures. This has resulted in an exponential increase in storage capacity while explaining the extensive memory, and it has the potential to illustrate the dynamics of neurons in the human brain when viewed from quantum mechanics perspective although the application of QHAM is limited as an autoassociation. We introduce a quantum-inspired multidirectional associative memory (QMAM) with a one-shot learning model, and QMAM with a self-convergent iterative learning model (IQMAM) based on QHAM in this paper. The self-convergent iterative learning enables the network to progressively develop a resonance state, from inputs to outputs. The simulation experiments demonstrate the advantages of QMAM and IQMAM, especially the stability to recall reliability.

Single-photon absorption by single photosynthetic light-harvesting complexes

NASA Astrophysics Data System (ADS)

Chan, Herman C. H.; Gamel, Omar E.; Fleming, Graham R.; Whaley, K. Birgitta

2018-03-01

We provide a unified theoretical approach to the quantum dynamics of absorption of single photons and subsequent excitonic energy transfer in photosynthetic light-harvesting complexes. Our analysis combines a continuous mode < n > -photon quantum optical master equation for the chromophoric system with the hierarchy of equations of motion describing excitonic dynamics in presence of non-Markovian coupling to vibrations of the chromophores and surrounding protein. We apply the approach to simulation of absorption of single-photon coherent states by pigment-protein complexes containing between one and seven chromophores, and compare with results obtained by excitation using a thermal radiation field. We show that the values of excitation probability obtained under single-photon absorption conditions can be consistently related to bulk absorption cross-sections. Analysis of the timescale and efficiency of single-photon absorption by light-harvesting systems within this full quantum description of pigment-protein dynamics coupled to a quantum radiation field reveals a non-trivial dependence of the excitation probability and the excited state dynamics induced by exciton-phonon coupling during and subsequent to the pulse, on the bandwidth of the incident photon pulse. For bandwidths equal to the spectral bandwidth of Chlorophyll a, our results yield an estimation of an average time of ˜0.09 s for a single chlorophyll chromophore to absorb the energy equivalent of one (single-polarization) photon under irradiation by single-photon states at the intensity of sunlight.

Fast generating Greenberger-Horne-Zeilinger state via iterative interaction pictures

NASA Astrophysics Data System (ADS)

Huang, Bi-Hua; Chen, Ye-Hong; Wu, Qi-Cheng; Song, Jie; Xia, Yan

2016-10-01

We delve a little deeper into the construction of shortcuts to adiabatic passage for three-level systems by iterative interaction picture (multiple Schrödinger dynamics). As an application example, we use the deduced iterative based shortcuts to rapidly generate the Greenberger-Horne-Zeilinger (GHZ) state in a three-atom system with the help of quantum Zeno dynamics. Numerical simulation shows the dynamics designed by the iterative picture method is physically feasible and the shortcut scheme performs much better than that using the conventional adiabatic passage techniques. Also, the influences of various decoherence processes are discussed by numerical simulation and the results prove that the scheme is fast and robust against decoherence and operational imperfection.

Nonequilibrium Quantum Simulation in Circuit QED

NASA Astrophysics Data System (ADS)

Raftery, James John

Superconducting circuits have become a leading architecture for quantum computing and quantum simulation. In particular, the circuit QED framework leverages high coherence qubits and microwave resonators to construct systems realizing quantum optics models with exquisite precision. For example, the Jaynes-Cummings model has been the focus of significant theoretical interest as a means of generating photon-photon interactions. Lattices of such strongly correlated photons are an exciting new test bed for exploring non-equilibrium condensed matter physics such as dissipative phase transitions of light. This thesis covers a series of experiments which establish circuit QED as a powerful tool for exploring condensed matter physics with photons. The first experiment explores the use of ultra high speed arbitrary waveform generators for the direct digital synthesis of complex microwave waveforms. This new technique dramatically simplifies the classical control chain for quantum experiments and enables high bandwidth driving schemes expected to be essential for generating interesting steady-states and dynamical behavior. The last two experiments explore the rich physics of interacting photons, with an emphasis on small systems where a high degree of control is possible. The first experiment realizes a two-site system called the Jaynes-Cummings dimer, which undergoes a self-trapping transition where the strong photon-photon interactions block photon hopping between sites. The observation of this dynamical phase transition and the related dissipation-induced transition are key results of this thesis. The final experiment augments the Jaynes-Cummings dimer by redesigning the circuit to include in-situ control over photon hopping between sites using a tunable coupler. This enables the study of the dimer's localization transition in the steady-state regime.

An Assessment of Molecular Dynamic Force Fields for Silica for Use in Simulating Laser Damage Mitigation

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

Soules, T F; Gilmer, G H; Matthews, M J

2010-10-21

We compare force fields (FF's) that have been used in molecular dynamic (MD) simulations of silica in order to assess their applicability for use in simulating IR-laser damage mitigation. Although pairwise FF?s obtained by fitting quantum mechanical calculations such as the BKS and CHIK potentials have been shown to reproduce many of the properties of silica including the stability of silica polymorphs and the densification of the liquid, we show that melting temperatures and fictive temperatures are much too high. Softer empirical force fields give liquid and glass properties at experimental temperatures but may not predict all properties important tomore » laser mitigation experiments.« less

Reduced quantum dynamics with arbitrary bath spectral densities: hierarchical equations of motion based on several different bath decomposition schemes.

PubMed

Liu, Hao; Zhu, Lili; Bai, Shuming; Shi, Qiang

2014-04-07

We investigated applications of the hierarchical equation of motion (HEOM) method to perform high order perturbation calculations of reduced quantum dynamics for a harmonic bath with arbitrary spectral densities. Three different schemes are used to decompose the bath spectral density into analytical forms that are suitable to the HEOM treatment: (1) The multiple Lorentzian mode model that can be obtained by numerically fitting the model spectral density. (2) The combined Debye and oscillatory Debye modes model that can be constructed by fitting the corresponding classical bath correlation function. (3) A new method that uses undamped harmonic oscillator modes explicitly in the HEOM formalism. Methods to extract system-bath correlations were investigated for the above bath decomposition schemes. We also show that HEOM in the undamped harmonic oscillator modes can give detailed information on the partial Wigner transform of the total density operator. Theoretical analysis and numerical simulations of the spin-Boson dynamics and the absorption line shape of molecular dimers show that the HEOM formalism for high order perturbations can serve as an important tool in studying the quantum dissipative dynamics in the intermediate coupling regime.

Reduced quantum dynamics with arbitrary bath spectral densities: Hierarchical equations of motion based on several different bath decomposition schemes

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

Liu, Hao; Zhu, Lili; Bai, Shuming

2014-04-07

We investigated applications of the hierarchical equation of motion (HEOM) method to perform high order perturbation calculations of reduced quantum dynamics for a harmonic bath with arbitrary spectral densities. Three different schemes are used to decompose the bath spectral density into analytical forms that are suitable to the HEOM treatment: (1) The multiple Lorentzian mode model that can be obtained by numerically fitting the model spectral density. (2) The combined Debye and oscillatory Debye modes model that can be constructed by fitting the corresponding classical bath correlation function. (3) A new method that uses undamped harmonic oscillator modes explicitly inmore » the HEOM formalism. Methods to extract system-bath correlations were investigated for the above bath decomposition schemes. We also show that HEOM in the undamped harmonic oscillator modes can give detailed information on the partial Wigner transform of the total density operator. Theoretical analysis and numerical simulations of the spin-Boson dynamics and the absorption line shape of molecular dimers show that the HEOM formalism for high order perturbations can serve as an important tool in studying the quantum dissipative dynamics in the intermediate coupling regime.« less

Entanglement of spin waves among four quantum memories.

PubMed

Choi, K S; Goban, A; Papp, S B; van Enk, S J; Kimble, H J

2010-11-18

Quantum networks are composed of quantum nodes that interact coherently through quantum channels, and open a broad frontier of scientific opportunities. For example, a quantum network can serve as a 'web' for connecting quantum processors for computation and communication, or as a 'simulator' allowing investigations of quantum critical phenomena arising from interactions among the nodes mediated by the channels. The physical realization of quantum networks generically requires dynamical systems capable of generating and storing entangled states among multiple quantum memories, and efficiently transferring stored entanglement into quantum channels for distribution across the network. Although such capabilities have been demonstrated for diverse bipartite systems, entangled states have not been achieved for interconnects capable of 'mapping' multipartite entanglement stored in quantum memories to quantum channels. Here we demonstrate measurement-induced entanglement stored in four atomic memories; user-controlled, coherent transfer of the atomic entanglement to four photonic channels; and characterization of the full quadripartite entanglement using quantum uncertainty relations. Our work therefore constitutes an advance in the distribution of multipartite entanglement across quantum networks. We also show that our entanglement verification method is suitable for studying the entanglement order of condensed-matter systems in thermal equilibrium.

Fast Model Generalized Pseudopotential Theory Interatomic Potential Routine

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

2015-03-18

MGPT is an unclassified source code for the fast evaluation and application of quantum-based MGPT interatomic potentials for mrtals. The present version of MGPT has been developed entirely at LLNL, but is specifically designed for implementation in the open-source molecular0dynamics code LAMMPS maintained by Sandia National Laboratories. Using MGPT in LAMMPS, with separate input potential data, one can perform large-scale atomistic simulations of the structural, thermodynamic, defeat and mechanical properties of transition metals with quantum-mechanical realism.

Towards ab initio Calculations with the Dynamical Vertex Approximation

NASA Astrophysics Data System (ADS)

Galler, Anna; Kaufmann, Josef; Gunacker, Patrik; Pickem, Matthias; Thunström, Patrik; Tomczak, Jan M.; Held, Karsten

2018-04-01

While key effects of the many-body problem — such as Kondo and Mott physics — can be understood in terms of on-site correlations, non-local fluctuations of charge, spin, and pairing amplitudes are at the heart of the most fascinating and unresolved phenomena in condensed matter physics. Here, we review recent progress in diagrammatic extensions to dynamical mean-field theory for ab initio materials calculations. We first recapitulate the quantum field theoretical background behind the two-particle vertex. Next we discuss latest algorithmic advances in quantum Monte Carlo simulations for calculating such two-particle quantities using worm sampling and vertex asymptotics, before giving an introduction to the ab initio dynamical vertex approximation (AbinitioDΓA). Finally, we highlight the potential of AbinitioDΓA by detailing results for the prototypical correlated metal SrVO3.

Role of quantum statistics in multi-particle decay dynamics

NASA Astrophysics Data System (ADS)

Marchewka, Avi; Granot, Er'el

2015-04-01

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

Perturbed path integrals in imaginary time: Efficiently modeling nuclear quantum effects in molecules and materials

NASA Astrophysics Data System (ADS)

Poltavsky, Igor; DiStasio, Robert A.; Tkatchenko, Alexandre

2018-03-01

Nuclear quantum effects (NQE), which include both zero-point motion and tunneling, exhibit quite an impressive range of influence over the equilibrium and dynamical properties of molecules and materials. In this work, we extend our recently proposed perturbed path-integral (PPI) approach for modeling NQE in molecular systems [I. Poltavsky and A. Tkatchenko, Chem. Sci. 7, 1368 (2016)], which successfully combines the advantages of thermodynamic perturbation theory with path-integral molecular dynamics (PIMD), in a number of important directions. First, we demonstrate the accuracy, performance, and general applicability of the PPI approach to both molecules and extended (condensed-phase) materials. Second, we derive a series of estimators within the PPI approach to enable calculations of structural properties such as radial distribution functions (RDFs) that exhibit rapid convergence with respect to the number of beads in the PIMD simulation. Finally, we introduce an effective nuclear temperature formalism within the framework of the PPI approach and demonstrate that such effective temperatures can be an extremely useful tool in quantitatively estimating the "quantumness" associated with different degrees of freedom in the system as well as providing a reliable quantitative assessment of the convergence of PIMD simulations. Since the PPI approach only requires the use of standard second-order imaginary-time PIMD simulations, these developments enable one to include a treatment of NQE in equilibrium thermodynamic properties (such as energies, heat capacities, and RDFs) with the accuracy of higher-order methods but at a fraction of the computational cost, thereby enabling first-principles modeling that simultaneously accounts for the quantum mechanical nature of both electrons and nuclei in large-scale molecules and materials.

Molecular Studies of Complex Soil Organic Matter Interactions with Metal Ions and Mineral Surfaces using Classical Molecular Dynamics and Quantum Chemistry Methods

NASA Astrophysics Data System (ADS)

Andersen, A.; Govind, N.; Laskin, A.

2017-12-01

Mineral surfaces have been implicated as potential protectors of soil organic matter (SOM) against decomposition and ultimate mineralization to small molecules which can provide nutrients for plants and soil microbes and can also contribute to the Earth's elemental cycles. SOM is a complex mixture of organic molecules of biological origin at varying degrees of decomposition and can, itself, self-assemble in such a way as to expose some biomolecule types to biotic and abiotic attack while protecting other biomolecule types. The organization of SOM and SOM with mineral surfaces and solvated metal ions is driven by an interplay of van der Waals and electrostatic interactions leading to partitioning of hydrophilic (e.g. sugars) and hydrophobic (e.g., lipids) SOM components that can be bridged with amphiphilic molecules (e.g., proteins). Classical molecular dynamics simulations can shed light on assemblies of organic molecules alone or complexation with mineral surfaces. The role of chemical reactions is also an important consideration in potential chemical changes of the organic species such as oxidation/reduction, degradation, chemisorption to mineral surfaces, and complexation with solvated metal ions to form organometallic systems. For the study of chemical reactivity, quantum chemistry methods can be employed and combined with structural insight provided by classical MD simulations. Moreover, quantum chemistry can also simulate spectroscopic signatures based on chemical structure and is a valuable tool in interpreting spectra from, notably, x-ray absorption spectroscopy (XAS). In this presentation, we will discuss our classical MD and quantum chemistry findings on a model SOM system interacting with mineral surfaces and solvated metal ions.

Quantum fluids of light in acoustic lattices

NASA Astrophysics Data System (ADS)

Cerda-Méndez, E. A.; Krizhanovskii, D. N.; Skolnick, M. S.; Santos, P. V.

2018-01-01

In this topical review, we report on the recent advances on the manipulation of hybrid light-matter quasi-particles called exciton-polaritons and their quantum condensed phases by means of acoustic and static periodic potentials. Polaritons are a superposition of photons and excitons and form in optical microcavities with quantum wells embedded in it. They are low-mass bosons in the dilute limit and have strong inter-particle interactions inherited from the excitonic component. Their capability to form quantum-condensed phases at temperatures in the kelvin range and to behave like quantum fluids makes them very attractive for novel solid-state devices. Since their de Broglie wavelength is of the order of a few micrometers, polaritons can be manipulated using static or dynamic potentials with micrometer scales. We present here a summary of the techniques used to submit polaritons and their condensed phases to periodic potentials, with an emphasis in dynamic ones produced by surface acoustic waves. We discuss the interesting phenomena that occur under such a modulation, such as condensation in excited states of the Brillouin zone, fragmentation of a condensate, formation of self-localized wavepackets, and Dirac and massive polaritons in static hexagonal and kagome lattices, respectively. The different techniques explored open the way to implement polariton-based quantum simulators, nano-optomechanic resonators and polaritonic topological insulators.

Accelerated quantum control using superadiabatic dynamics in a solid-state lambda system

DOE PAGES

Zhou, Brian B.; Baksic, Alexandre; Ribeiro, Hugo; ...

2016-11-28

Adiabatic evolutions find widespread utility in applications to quantum state engineering1 , geometric quantum computation2 , and quantum simulation3 . Although offering desirable robustness to experimental imperfections, adiabatic techniques are susceptible to decoherence during their long operation time. A recent strategy termed ‘shortcuts to adiabaticity’ 4–10 (STA) aims to circumvent this trade-off by designing fast dynamics to reproduce the results of infinitely slow, adiabatic processes. Here, as a realization of this strategy, we implement ‘superadiabatic’ transitionless driving11 (SATD) to speed up stimulated Raman adiabatic passage1,12–15 (STIRAP) in a solid-state lambda (Λ) system. Utilizing optical transitions to a dissipative excited statemore » in the nitrogen vacancy (NV) center in diamond, we demonstrate the accelerated performance of different shortcut trajectories for population transfer and for the transfer and initialization of coherent superpositions. We reveal that SATD protocols exhibit robustness to dissipation and experimental uncertainty, and can be optimized when these effects are present. These results motivate STA as a promising tool for controlling open quantum systems comprising individual or hybrid nanomechanical, superconducting, and photonic elements in the solid state12–17.« less

Quantum simulation of the spin-boson model with a microwave circuit

NASA Astrophysics Data System (ADS)

Leppäkangas, Juha; Braumüller, Jochen; Hauck, Melanie; Reiner, Jan-Michael; Schwenk, Iris; Zanker, Sebastian; Fritz, Lukas; Ustinov, Alexey V.; Weides, Martin; Marthaler, Michael

2018-05-01

We consider superconducting circuits for the purpose of simulating the spin-boson model. The spin-boson model consists of a single two-level system coupled to bosonic modes. In most cases, the model is considered in a limit where the bosonic modes are sufficiently dense to form a continuous spectral bath. A very well known case is the Ohmic bath, where the density of states grows linearly with the frequency. In the limit of weak coupling or large temperature, this problem can be solved numerically. If the coupling is strong, the bosonic modes can become sufficiently excited to make a classical simulation impossible. Here we discuss how a quantum simulation of this problem can be performed by coupling a superconducting qubit to a set of microwave resonators. We demonstrate a possible implementation of a continuous spectral bath with individual bath resonators coupling strongly to the qubit. Applying a microwave drive scheme potentially allows us to access the strong-coupling regime of the spin-boson model. We discuss how the resulting spin relaxation dynamics with different initialization conditions can be probed by standard qubit-readout techniques from circuit quantum electrodynamics.

Quantum simulations and many-body physics with light.

PubMed

Noh, Changsuk; Angelakis, Dimitris G

2017-01-01

In this review we discuss the works in the area of quantum simulation and many-body physics with light, from the early proposals on equilibrium models to the more recent works in driven dissipative platforms. We start by describing the founding works on Jaynes-Cummings-Hubbard model and the corresponding photon-blockade induced Mott transitions and continue by discussing the proposals to simulate effective spin models and fractional quantum Hall states in coupled resonator arrays (CRAs). We also analyse the recent efforts to study out-of-equilibrium many-body effects using driven CRAs, including the predictions for photon fermionisation and crystallisation in driven rings of CRAs as well as other dynamical and transient phenomena. We try to summarise some of the relatively recent results predicting exotic phases such as super-solidity and Majorana like modes and then shift our attention to developments involving 1D nonlinear slow light setups. There the simulation of strongly correlated phases characterising Tonks-Girardeau gases, Luttinger liquids, and interacting relativistic fermionic models is described. We review the major theory results and also briefly outline recent developments in ongoing experimental efforts involving different platforms in circuit QED, photonic crystals and nanophotonic fibres interfaced with cold atoms.

Quantum magnetism in different AMO systems.

NASA Astrophysics Data System (ADS)

Rey, Ana Maria

One of the most important goals of modern quantum sciences is to learn how to control and entangle many-body systems and use them to make powerful and improved quantum devices, materials and technologies. However, since performing full state tomography does not scale favorably with the number of particles, as the size of quantum systems grow, it becomes extremely challenging to identify, and quantify the buildup of quantum correlations and coherence. In this talk I will report on a protocol that we have developed and experimentally demonstrated in a trapped ion quantum magnet in a Penning trap, which can perform quantum simulations of Ising spin models. In those experiments strong spin-spin interactions can be engineered through optical dipole forces that excite phonons of the crystals. The number of ions can be varied from tens to hundreds with high fidelity control. The protocol uses time reversal of the many-body dynamics, to measure out-of-time-order correlation functions (OTOCs). By measuring a family of OTOCs as a function of a tunable parameter we obtain fine-grained information about the state of the system encoded in the multiple quantum coherence spectrum, extract the quantum state purity, and demonstrate the build-up of up to 8-body correlations. We also use the protocol and comparisons to a full solution of the master equation to investigate the impact of spin-motion entanglement and decoherence in the quantum dynamics. Future applications of this protocol could enable studies of manybody localization, quantum phase transitions, and tests of the holographic duality between quantum and gravitational systems. Supported by NSF-PHY-1521080, JILA-NSF PFC-1125844, ARO and AFOSR-MURI.

Nonconservative dynamics in long atomic wires

NASA Astrophysics Data System (ADS)

Cunningham, Brian; Todorov, Tchavdar N.; Dundas, Daniel

2014-09-01

The effect of nonconservative current-induced forces on the ions in a defect-free metallic nanowire is investigated using both steady-state calculations and dynamical simulations. Nonconservative forces were found to have a major influence on the ion dynamics in these systems, but their role in increasing the kinetic energy of the ions decreases with increasing system length. The results illustrate the importance of nonconservative effects in short nanowires and the scaling of these effects with system size. The dependence on bias and ion mass can be understood with the help of a simple pen and paper model. This material highlights the benefit of simple preliminary steady-state calculations in anticipating aspects of brute-force dynamical simulations, and provides rule of thumb criteria for the design of stable quantum wires.

First-principles simulations of heat transport

NASA Astrophysics Data System (ADS)

Puligheddu, Marcello; Gygi, Francois; Galli, Giulia

2017-11-01

Advances in understanding heat transport in solids were recently reported by both experiment and theory. However an efficient and predictive quantum simulation framework to investigate thermal properties of solids, with the same complexity as classical simulations, has not yet been developed. Here we present a method to compute the thermal conductivity of solids by performing ab initio molecular dynamics at close to equilibrium conditions, which only requires calculations of first-principles trajectories and atomic forces, thus avoiding direct computation of heat currents and energy densities. In addition the method requires much shorter sequential simulation times than ordinary molecular dynamics techniques, making it applicable within density functional theory. We discuss results for a representative oxide, MgO, at different temperatures and for ordered and nanostructured morphologies, showing the performance of the method in different conditions.

Quantum entanglement in strong-field ionization

NASA Astrophysics Data System (ADS)

Majorosi, Szilárd; Benedict, Mihály G.; Czirják, Attila

2017-10-01

We investigate the time evolution of quantum entanglement between an electron, liberated by a strong few-cycle laser pulse, and its parent ion core. Since the standard procedure is numerically prohibitive in this case, we propose a method to quantify the quantum correlation in such a system: we use the reduced density matrices of the directional subspaces along the polarization of the laser pulse and along the transverse directions as building blocks for an approximate entanglement entropy. We present our results, based on accurate numerical simulations, in terms of several of these entropies, for selected values of the peak electric-field strength and the carrier-envelope phase difference of the laser pulse. The time evolution of the mutual entropy of the electron and the ion-core motion along the direction of the laser polarization is similar to our earlier results based on a simple one-dimensional model. However, taking into account also the dynamics perpendicular to the laser polarization reveals a surprisingly different entanglement dynamics above the laser intensity range corresponding to pure tunneling: the quantum entanglement decreases with time in the over-the-barrier ionization regime.

Shortcuts to adiabaticity using flow fields

NASA Astrophysics Data System (ADS)

Patra, Ayoti; Jarzynski, Christopher

2017-12-01

A shortcut to adiabaticity is a recipe for generating adiabatic evolution at an arbitrary pace. Shortcuts have been developed for quantum, classical and (most recently) stochastic dynamics. A shortcut might involve a counterdiabatic (CD) Hamiltonian that causes a system to follow the adiabatic evolution at all times, or it might utilize a fast-forward (FF) potential, which returns the system to the adiabatic path at the end of the process. We develop a general framework for constructing shortcuts to adiabaticity from flow fields that describe the desired adiabatic evolution. Our approach encompasses quantum, classical and stochastic dynamics, and provides surprisingly compact expressions for both CD Hamiltonians and FF potentials. We illustrate our method with numerical simulations of a model system, and we compare our shortcuts with previously obtained results. We also consider the semiclassical connections between our quantum and classical shortcuts. Our method, like the FF approach developed by previous authors, is susceptible to singularities when applied to excited states of quantum systems; we propose a simple, intuitive criterion for determining whether these singularities will arise, for a given excited state.

Zero-Point Energy Leakage in Quantum Thermal Bath Molecular Dynamics Simulations.

PubMed

Brieuc, Fabien; Bronstein, Yael; Dammak, Hichem; Depondt, Philippe; Finocchi, Fabio; Hayoun, Marc

2016-12-13

The quantum thermal bath (QTB) has been presented as an alternative to path-integral-based methods to introduce nuclear quantum effects in molecular dynamics simulations. The method has proved to be efficient, yielding accurate results for various systems. However, the QTB method is prone to zero-point energy leakage (ZPEL) in highly anharmonic systems. This is a well-known problem in methods based on classical trajectories where part of the energy of the high-frequency modes is transferred to the low-frequency modes leading to a wrong energy distribution. In some cases, the ZPEL can have dramatic consequences on the properties of the system. Thus, we investigate the ZPEL by testing the QTB method on selected systems with increasing complexity in order to study the conditions and the parameters that influence the leakage. We also analyze the consequences of the ZPEL on the structural and vibrational properties of the system. We find that the leakage is particularly dependent on the damping coefficient and that increasing its value can reduce and, in some cases, completely remove the ZPEL. When using sufficiently high values for the damping coefficient, the expected energy distribution among the vibrational modes is ensured. In this case, the QTB method gives very encouraging results. In particular, the structural properties are well-reproduced. The dynamical properties should be regarded with caution although valuable information can still be extracted from the vibrational spectrum, even for large values of the damping term.

Cis-trans photoisomerization of azobenzene upon excitation to the S1 state: an ab initio molecular dynamics and QM/MM study

NASA Astrophysics Data System (ADS)

Pederzoli, Marek; Pittner, Jiří; Barbatti, Mario; Lischka, Hans

2012-10-01

The cis-trans isomerization of azobenzene upon S1(n,π*) excitation is studied both in gas phase and in solution. Our study is based on ab initio non-adiabatic dynamics simulations with the non-adiabatic effects included via the fewest-switches surface hopping method with potential-energy surfaces and couplings determined on the fly. The non-adiabatic couplings have been computed based on overlaps of CASSCF wave functions. The solvent is described using classical molecular dynamics employing the quantum mechanics/molecular mechanics (QM/MM) approach. Azobenzene photoisomerization upon S1(n,π*) excitation occurs purely as a rotational motion of the central CNNC moiety. Two non-equivalent rotational pathways, corresponding to clockwise or counterclockwise rotation, are available. The course of the rotational motion is strongly dependent on the initial conditions. The internal conversion occurs via a S0/S1 crossing seam located near the midpoint of both of these rotational pathways. Based on statistical analysis it is shown that the occurrence of one or other pathways can be completely controlled by selecting adequate initial conditions. The effect of the solvent on the reaction mechanism is small. The lifetime of the S1 state is marginally lowered; the effect does not depend on the polarity, but rather on the viscosity of the solvent. The quantum yield is solvent dependent; the simulations in water give smaller quantum yield than those obtained in n-hexane and in gas phase.

Computational approach on PEB process in EUV resist: multi-scale simulation

NASA Astrophysics Data System (ADS)

Kim, Muyoung; Moon, Junghwan; Choi, Joonmyung; Lee, Byunghoon; Jeong, Changyoung; Kim, Heebom; Cho, Maenghyo

2017-03-01

For decades, downsizing has been a key issue for high performance and low cost of semiconductor, and extreme ultraviolet lithography is one of the promising candidates to achieve the goal. As a predominant process in extreme ultraviolet lithography on determining resolution and sensitivity, post exposure bake has been mainly studied by experimental groups, but development of its photoresist is at the breaking point because of the lack of unveiled mechanism during the process. Herein, we provide theoretical approach to investigate underlying mechanism on the post exposure bake process in chemically amplified resist, and it covers three important reactions during the process: acid generation by photo-acid generator dissociation, acid diffusion, and deprotection. Density functional theory calculation (quantum mechanical simulation) was conducted to quantitatively predict activation energy and probability of the chemical reactions, and they were applied to molecular dynamics simulation for constructing reliable computational model. Then, overall chemical reactions were simulated in the molecular dynamics unit cell, and final configuration of the photoresist was used to predict the line edge roughness. The presented multiscale model unifies the phenomena of both quantum and atomic scales during the post exposure bake process, and it will be helpful to understand critical factors affecting the performance of the resulting photoresist and design the next-generation material.

Exploration of bulk and interface behavior of gas molecules and 1-butyl-3-methylimidazolium tetrafluoroborate ionic liquid using equilibrium and nonequilibrium molecular dynamics simulation and quantum chemical calculation.

PubMed

Yang, Quan; Achenie, Luke E K

2018-04-18

Ionic liquids (ILs) show brilliant performance in separating gas impurities, but few researchers have performed an in-depth exploration of the bulk and interface behavior of penetrants and ILs thoroughly. In this research, we have performed a study on both molecular dynamics (MD) simulation and quantum chemical (QC) calculation to explore the transport of acetylene and ethylene in the bulk and interface regions of 1-butyl-3-methylimidazolium tetrafluoroborate ([BMIM]-[BF4]). The diffusivity, solubility and permeability of gas molecules in the bulk were researched with MD simulation first. The subdiffusion behavior of gas molecules is induced by coupling between the motion of gas molecules and the ions, and the relaxation processes of the ions after the disturbance caused by gas molecules. Then, QC calculation was performed to explore the optical geometry of ions, ion pairs and complexes of ions and penetrants, and interaction potential for pairs and complexes. Finally, nonequilibrium MD simulation was performed to explore the interface structure and properties of the IL-gas system and gas molecule behavior in the interface region. The research results may be used in the design of IL separation media.

Entropy, energy, and entanglement of localized states in bent triatomic molecules

NASA Astrophysics Data System (ADS)

Yuan, Qiang; Hou, Xi-Wen

2017-05-01

The dynamics of quantum entropy, energy, and entanglement is studied for various initial states in an important spectroscopic Hamiltonian of bent triatomic molecules H2O, D2O, and H2S. The total quantum correlation is quantified in terms of the mutual information and the entanglement by the concurrence borrowed from the theory of quantum information. The Pauli entropy and the intramolecular energy usually used in the theory of molecules are calculated to establish a possible relationship between both theories. Sections of two quantities among these four quantities are introduced to visualize such relationship. Analytic and numerical simulations demonstrate that if an initial state is taken to be the stretch- or the bend-vibrationally localized state, the mutual information, the Pauli entropy, and the concurrence are dominant-positively correlated while they are dominantly anti-correlated with the interacting energy among three anharmonic vibrational modes. In particular, such correlation is more distinct for the localized state with high excitations in the bending mode. The nice quasi-periodicity of those quantities in D2O molecule reveals that this molecule prepared in the localized state in the stretching or the bending mode can be more appreciated for molecular quantum computation. However, the dynamical correlations of those quantities behave irregularly for the dislocalized states. Moreover, the hierarchy of the mutual information and the Pauli entropy is explicitly proved. Quantum entropy and energy in every vibrational mode are investigated. Thereby, the relation between bipartite and tripartite entanglements is discussed as well. Those are useful for the understanding of quantum correlations in high-dimensional states in polyatomic molecules from quantum information and intramolecular dynamics.

New insights into the nonadiabatic state population dynamics of model proton-coupled electron transfer reactions from the mixed quantum-classical Liouville approach

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

Shakib, Farnaz A.; Hanna, Gabriel, E-mail: gabriel.hanna@ualberta.ca

In a previous study [F. A. Shakib and G. Hanna, J. Chem. Phys. 141, 044122 (2014)], we investigated a model proton-coupled electron transfer (PCET) reaction via the mixed quantum-classical Liouville (MQCL) approach and found that the trajectories spend the majority of their time on the mean of two coherently coupled adiabatic potential energy surfaces. This suggested a need for mean surface evolution to accurately simulate observables related to ultrafast PCET processes. In this study, we simulate the time-dependent populations of the three lowest adiabatic states in the ET-PT (i.e., electron transfer preceding proton transfer) version of the same PCET modelmore » via the MQCL approach and compare them to the exact quantum results and those obtained via the fewest switches surface hopping (FSSH) approach. We find that the MQCL population profiles are in good agreement with the exact quantum results and show a significant improvement over the FSSH results. All of the mean surfaces are shown to play a direct role in the dynamics of the state populations. Interestingly, our results indicate that the population transfer to the second-excited state can be mediated by dynamics on the mean of the ground and second-excited state surfaces, as part of a sequence of nonadiabatic transitions that bypasses the first-excited state surface altogether. This is made possible through nonadiabatic transitions between different mean surfaces, which is the manifestation of coherence transfer in MQCL dynamics. We also investigate the effect of the strength of the coupling between the proton/electron and the solvent coordinate on the state population dynamics. Drastic changes in the population dynamics are observed, which can be understood in terms of the changes in the potential energy surfaces and the nonadiabatic couplings. Finally, we investigate the state population dynamics in the PT-ET (i.e., proton transfer preceding electron transfer) and concerted versions of the model. The PT-ET results confirm the participation of all of the mean surfaces, albeit in different proportions compared to the ET-PT case, while the concerted results indicate that the mean of the ground- and first-excited state surfaces only plays a role, due to the large energy gaps between the ground- and second-excited state surfaces.« less

Exploring the quantum critical behaviour in a driven Tavis–Cummings circuit

PubMed Central

Feng, M.; Zhong, Y.P.; Liu, T.; Yan, L.L.; Yang, W.L.; Twamley, J.; Wang, H.

2015-01-01

Quantum phase transitions play an important role in many-body systems and have been a research focus in conventional condensed-matter physics over the past few decades. Artificial atoms, such as superconducting qubits that can be individually manipulated, provide a new paradigm of realising and exploring quantum phase transitions by engineering an on-chip quantum simulator. Here we demonstrate experimentally the quantum critical behaviour in a highly controllable superconducting circuit, consisting of four qubits coupled to a common resonator mode. By off-resonantly driving the system to renormalize the critical spin-field coupling strength, we have observed a four-qubit nonequilibrium quantum phase transition in a dynamical manner; that is, we sweep the critical coupling strength over time and monitor the four-qubit scaled moments for a signature of a structural change of the system's eigenstates. Our observation of the nonequilibrium quantum phase transition, which is in good agreement with the driven Tavis–Cummings theory under decoherence, offers new experimental approaches towards exploring quantum phase transition-related science, such as scaling behaviours, parity breaking and long-range quantum correlations. PMID:25971985

Fidelity Witnesses for Fermionic Quantum Simulations

NASA Astrophysics Data System (ADS)

Gluza, M.; Kliesch, M.; Eisert, J.; Aolita, L.

2018-05-01

The experimental interest and developments in quantum spin-1 /2 chains has increased uninterruptedly over the past decade. In many instances, the target quantum simulation belongs to the broader class of noninteracting fermionic models, constituting an important benchmark. In spite of this class being analytically efficiently tractable, no direct certification tool has yet been reported for it. In fact, in experiments, certification has almost exclusively relied on notions of quantum state tomography scaling very unfavorably with the system size. Here, we develop experimentally friendly fidelity witnesses for all pure fermionic Gaussian target states. Their expectation value yields a tight lower bound to the fidelity and can be measured efficiently. We derive witnesses in full generality in the Majorana-fermion representation and apply them to experimentally relevant spin-1 /2 chains. Among others, we show how to efficiently certify strongly out-of-equilibrium dynamics in critical Ising chains. At the heart of the measurement scheme is a variant of importance sampling specially tailored to overlaps between covariance matrices. The method is shown to be robust against finite experimental-state infidelities.

Quantum Engineering of Dynamical Gauge Fields on Optical Lattices

DTIC Science & Technology

2016-07-08

exact blocking formulas from the TRG formulation of the transfer matrix. The second is a worm algorithm. The particle number distributions obtained...a fact that can be explained by an approximate particle- hole symmetry. We have also developed a computer code suite for simulating the Abelian

Application of JAERI quantum molecular dynamics model for collisions of heavy nuclei

NASA Astrophysics Data System (ADS)

Ogawa, Tatsuhiko; Hashimoto, Shintaro; Sato, Tatsuhiko; Niita, Koji

2016-06-01

The quantum molecular dynamics (QMD) model incorporated into the general-purpose radiation transport code PHITS was revised for accurate prediction of fragment yields in peripheral collisions. For more accurate simulation of peripheral collisions, stability of the nuclei at their ground state was improved and the algorithm to reject invalid events was modified. In-medium correction on nucleon-nucleon cross sections was also considered. To clarify the effect of this improvement on fragmentation of heavy nuclei, the new QMD model coupled with a statistical decay model was used to calculate fragment production cross sections of Ag and Au targets and compared with the data of earlier measurement. It is shown that the revised version can predict cross section more accurately.

A classical phase r-centroid approach to molecular wave packet dynamics illustrating the danger of using an incomplete set of initial states for thermal averaging

NASA Astrophysics Data System (ADS)

Hansson, Tony

1999-08-01

An inexpensive semiclassical method to simulate time-resolved pump-probe spectroscopy on molecular wave packets is applied to NaK molecules at high temperature. The method builds on the introduction of classical phase factors related to the r-centroids for vibronic transitions and assumes instantaneous laser-molecule interaction. All observed quantum mechanical features are reproduced - for short times where experimental data are available even quantitatively. Furthermore, it is shown that fully quantum dynamical molecular wave packet calculations on molecules at elevated temperatures, which do not include all rovibrational states, must be regarded with caution, as they easily might yield even qualitatively incorrect results.

Investigation of Kibble-Zurek Quench Dynamics in a Spin-1 Ferromagnetic BEC

NASA Astrophysics Data System (ADS)

Anquez, Martin; Robbins, Bryce; Hoang, Thai; Yang, Xiaoyun; Land, Benjamin; Hamley, Christopher; Chapman, Michael

2014-05-01

We study the temporal evolution of spin populations in small spin-1 87Rb condensates following a slow quench. A ferromagnetic spin-1 BEC exhibits a second-order gapless (quantum) phase transition due to a competition between the magnetic and collisional spin interaction energies. The dynamics of slow quenches through the critical point are predicted to exhibit universal power-law scaling as a function of quench speed. In spatially extended condensates, these excitations are revealed as spatial spin domains. In small condensates, the excitations are manifest in the temporal evolution of the spin populations, illustrating a Kibble-Zurek type scaling. We will present the results of our investigation and compare them to full quantum simulations of the system.

Improvement on Fermionic properties and new isotope production in molecular dynamics simulations

NASA Astrophysics Data System (ADS)

Wang, Ning; Wu, Tong; Zeng, Jie; Yang, Yongxu; Ou, Li

2016-06-01

By considering momentum transfer in the Fermi constraint procedure, the stability of the initial nuclei and fragments produced in heavy-ion collisions can be further improved in quantum molecular dynamics simulations. The case of a phase-space occupation probability larger than one is effectively reduced with the proposed procedure. Simultaneously, the energy conservation can be better described for both individual nuclei and heavy-ion reactions. With the revised version of the improved quantum molecular dynamics model, the fusion excitation functions of 16O+186W and the central collisions of Au+Au at 35 AMeV are re-examined. The fusion cross sections at sub-barrier energies and the charge distribution of fragments are relatively better reproduced due to the reduction of spurious nucleon emission. The charge and isotope distribution of fragments in Xe+Sn, U+U and Zr+Sn at intermediate energies are also predicted. More unmeasured extremely neutron-rich fragments with Z = 16-28 are observed in the central collisions of 238U+238U than that of 96Zr+124Sn, which indicates that multi-fragmentation of U+U may offer a fruitful pathway to new neutron-rich isotopes.

How can we probe the atom mass currents induced by synthetic gauge fields?

NASA Astrophysics Data System (ADS)

Paramekanti, Arun; Killi, Matthew; Trotzky, Stefan

2013-05-01

Ultracold atomic fermions and bosons in an optical lattice can have quantum ground states which support equilibrium currents in the presence of synthetic magnetic fields or spin orbit coupling. As a tool to uncover these mass currents, we propose using an anisotropic quantum quench of the optical lattice which dynamically converts the current patterns into measurable density patterns. Using analytical calculations and numerical simulations, we show that this scheme can probe diverse equilibrium bulk current patterns in Bose superfluids and Fermi fluids induced by synthetic magnetic fields, as well as detect the chiral edge currents in topological states of atomic matter such as quantum Hall and quantum spin Hall insulators. This work is supported by NSERC of Canada and the Canadian Institute for Advanced Research.

Pechukas-Yukawa approach to the evolution of the quantum state of a parametrically perturbed system

NASA Astrophysics Data System (ADS)

Qureshi, Mumnuna A.; Zhong, Johnny; Qureshi, Zihad; Mason, Peter; Betouras, Joseph J.; Zagoskin, Alexandre M.

2018-03-01

We consider the evolution of the quantum states of a Hamiltonian that is parametrically perturbed via a term proportional to the adiabatic parameter λ (t ) . Starting with the Pechukas-Yukawa mapping of the energy eigenvalue evolution in a generalized Calogero-Sutherland model of a one-dimensional classical gas, we consider the adiabatic approximation with two different expansions of the quantum state in powers of d λ /d t and compare them with a direct numerical simulation. We show that one of these expansions (Magnus series) is especially convenient for the description of nonadiabatic evolution of the system. Applying the expansion to the exact cover 3-satisfiability problem, we obtain the occupation dynamics, which provides insight into the population of states and sources of decoherence in a quantum system.

InAs wetting layer and quantum dots on GaAs(001) surface studied by in situ STM placed inside MBE growth chamber and kMC simulations based on first-principles calculations

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

Tsukamoto, S.; Arakawa, Y.; Bell, G. R.

2007-04-10

Dynamic images of InAs quantum dots (QDs) formation are obtained using a unique scanning tunneling microscope (STM) placed within the growth chamber. These images are interpreted with the aid of kinetic Monte Carlo (kMC) simulations of the QD nucleation process. Alloy fluctuations in the InGaAs wetting layer prior to QD formation assist in the nucleation of stable InAs islands containing tens of atoms which grow extremely rapidly to form QDs. Furthermore, not all deposited In is initially incorporated into the lattice, providing a large supply of material to rapidly form QDs at the critical thickness.

Probing polariton dynamics in trapped ions with phase-coherent two-dimensional spectroscopy

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

Gessner, Manuel; Schlawin, Frank; Buchleitner, Andreas

2015-06-07

We devise a phase-coherent three-pulse protocol to probe the polariton dynamics in a trapped-ion quantum simulation. In contrast to conventional nonlinear signals, the presented scheme does not change the number of excitations in the system, allowing for the investigation of the dynamics within an N-excitation manifold. In the particular case of a filling factor one (N excitations in an N-ion chain), the proposed interaction induces coherent transitions between a delocalized phonon superfluid and a localized atomic insulator phase. Numerical simulations of a two-ion chain demonstrate that the resulting two-dimensional spectra allow for the unambiguous identification of the distinct phases, andmore » the two-dimensional line shapes efficiently characterize the relevant decoherence mechanism.« less

Revisiting structure and dynamics of preferential solvation of K(I) ion in aqueous ammonia using QMCF-MD simulation

NASA Astrophysics Data System (ADS)

Hidayat, Yuniawan; Pranowo, Harno Dwi; Armunanto, Ria

2018-05-01

Structure and dynamics of preferential solvation of K(I) ion in aqueous ammonia have been reinvestigated using ab initio quantum mechanical charge field (QMCF) molecular dynamics (MD) simulation. The average coordination number of the first solvation consists of 2 ammonia and 4 waters. The mean residence time is less than 2 ps confirming the rapid mobility of ligands. The distance evolution data shows the frequent of ligand exchanges. The second solvation shell shows a more labile structure. The NBO analysis of the first shell structure emphasizes that interaction of K(I)-H2O is stronger than K(I)-NH3. The Wiberg bond confirms a weak electrostatic of ion-ligand interaction.

First-principles quantum-mechanical investigations of biomass conversion at the liquid-solid interfaces

NASA Astrophysics Data System (ADS)

Dang, Hongli; Xue, Wenhua; Liu, Yingdi; Jentoft, Friederike; Resasco, Daniel; Wang, Sanwu

2014-03-01

We report first-principles density-functional calculations and ab initio molecular dynamics (MD) simulations for the reactions involving furfural, which is an important intermediate in biomass conversion, at the catalytic liquid-solid interfaces. The different dynamic processes of furfural at the water-Cu(111) and water-Pd(111) interfaces suggest different catalytic reaction mechanisms for the conversion of furfural. Simulations for the dynamic processes with and without hydrogen demonstrate the importance of the liquid-solid interface as well as the presence of hydrogen in possible catalytic reactions including hydrogenation and decarbonylation of furfural. Supported by DOE (DE-SC0004600). This research used the supercomputer resources of the XSEDE, the NERSC Center, and the Tandy Supercomputing Center.

Small slot waveguide rings for on-chip quantum optical circuits.

PubMed

Rotenberg, Nir; Türschmann, Pierre; Haakh, Harald R; Martin-Cano, Diego; Götzinger, Stephan; Sandoghdar, Vahid

2017-03-06

Nanophotonic interfaces between single emitters and light promise to enable new quantum optical technologies. Here, we use a combination of finite element simulations and analytic quantum theory to investigate the interaction of various quantum emitters with slot-waveguide rings. We predict that for rings with radii as small as 1.44 μm, with a Q-factor of 27,900, near-unity emitter-waveguide coupling efficiencies and emission enhancements on the order of 1300 can be achieved. By tuning the ring geometry or introducing losses, we show that realistic emitter-ring systems can be made to be either weakly or strongly coupled, so that we can observe Rabi oscillations in the decay dynamics even for micron-sized rings. Moreover, we demonstrate that slot waveguide rings can be used to directionally couple emission, again with near-unity efficiency. Our results pave the way for integrated solid-state quantum circuits involving various emitters.

Quantum simulator review

NASA Astrophysics Data System (ADS)

Bednar, Earl; Drager, Steven L.

2007-04-01

Quantum information processing's objective is to utilize revolutionary computing capability based on harnessing the paradigm shift offered by quantum computing to solve classically hard and computationally challenging problems. Some of our computationally challenging problems of interest include: the capability for rapid image processing, rapid optimization of logistics, protecting information, secure distributed simulation, and massively parallel computation. Currently, one important problem with quantum information processing is that the implementation of quantum computers is difficult to realize due to poor scalability and great presence of errors. Therefore, we have supported the development of Quantum eXpress and QuIDD Pro, two quantum computer simulators running on classical computers for the development and testing of new quantum algorithms and processes. This paper examines the different methods used by these two quantum computing simulators. It reviews both simulators, highlighting each simulators background, interface, and special features. It also demonstrates the implementation of current quantum algorithms on each simulator. It concludes with summary comments on both simulators.

Tunneling and speedup in quantum optimization for permutation-symmetric problems

DOE PAGES

Muthukrishnan, Siddharth; Albash, Tameem; Lidar, Daniel A.

2016-07-21

Tunneling is often claimed to be the key mechanism underlying possible speedups in quantum optimization via quantum annealing (QA), especially for problems featuring a cost function with tall and thin barriers. We present and analyze several counterexamples from the class of perturbed Hamming weight optimization problems with qubit permutation symmetry. We first show that, for these problems, the adiabatic dynamics that make tunneling possible should be understood not in terms of the cost function but rather the semiclassical potential arising from the spin-coherent path-integral formalism. We then provide an example where the shape of the barrier in the final costmore » function is short and wide, which might suggest no quantum advantage for QA, yet where tunneling renders QA superior to simulated annealing in the adiabatic regime. However, the adiabatic dynamics turn out not be optimal. Instead, an evolution involving a sequence of diabatic transitions through many avoided-level crossings, involving no tunneling, is optimal and outperforms adiabatic QA. We show that this phenomenon of speedup by diabatic transitions is not unique to this example, and we provide an example where it provides an exponential speedup over adiabatic QA. In yet another twist, we show that a classical algorithm, spin-vector dynamics, is at least as efficient as diabatic QA. Lastly, in a different example with a convex cost function, the diabatic transitions result in a speedup relative to both adiabatic QA with tunneling and classical spin-vector dynamics.« less

Tunneling and speedup in quantum optimization for permutation-symmetric problems

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

Muthukrishnan, Siddharth; Albash, Tameem; Lidar, Daniel A.

Tunneling is often claimed to be the key mechanism underlying possible speedups in quantum optimization via quantum annealing (QA), especially for problems featuring a cost function with tall and thin barriers. We present and analyze several counterexamples from the class of perturbed Hamming weight optimization problems with qubit permutation symmetry. We first show that, for these problems, the adiabatic dynamics that make tunneling possible should be understood not in terms of the cost function but rather the semiclassical potential arising from the spin-coherent path-integral formalism. We then provide an example where the shape of the barrier in the final costmore » function is short and wide, which might suggest no quantum advantage for QA, yet where tunneling renders QA superior to simulated annealing in the adiabatic regime. However, the adiabatic dynamics turn out not be optimal. Instead, an evolution involving a sequence of diabatic transitions through many avoided-level crossings, involving no tunneling, is optimal and outperforms adiabatic QA. We show that this phenomenon of speedup by diabatic transitions is not unique to this example, and we provide an example where it provides an exponential speedup over adiabatic QA. In yet another twist, we show that a classical algorithm, spin-vector dynamics, is at least as efficient as diabatic QA. Lastly, in a different example with a convex cost function, the diabatic transitions result in a speedup relative to both adiabatic QA with tunneling and classical spin-vector dynamics.« less

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.

Eigenstates and dynamics of Hooke's atom: Exact results and path integral simulations

NASA Astrophysics Data System (ADS)

Gholizadehkalkhoran, Hossein; Ruokosenmäki, Ilkka; Rantala, Tapio T.

2018-05-01

The system of two interacting electrons in one-dimensional harmonic potential or Hooke's atom is considered, again. On one hand, it appears as a model for quantum dots in a strong confinement regime, and on the other hand, it provides us with a hard test bench for new methods with the "space splitting" arising from the one-dimensional Coulomb potential. Here, we complete the numerous previous studies of the ground state of Hooke's atom by including the excited states and dynamics, not considered earlier. With the perturbation theory, we reach essentially exact eigenstate energies and wave functions for the strong confinement regime as novel results. We also consider external perturbation induced quantum dynamics in a simple separable case. Finally, we test our novel numerical approach based on real-time path integrals (RTPIs) in reproducing the above. The RTPI turns out to be a straightforward approach with exact account of electronic correlations for solving the eigenstates and dynamics without the conventional restrictions of electronic structure methods.

Refinement of the experimental dynamic structure factor for liquid para-hydrogen and ortho-deuterium using semi-classical quantum simulation.

PubMed

Smith, Kyle K G; Poulsen, Jens Aage; Cunsolo, A; Rossky, Peter J

2014-01-21

The dynamic structure factor of liquid para-hydrogen and ortho-deuterium in corresponding thermodynamic states (T = 20.0 K, n = 21.24 nm(-3)) and (T = 23.0 K, n = 24.61 nm(-3)), respectively, has been computed by both the Feynman-Kleinert linearized path-integral (FK-LPI) and Ring-Polymer Molecular Dynamics (RPMD) methods and compared with Inelastic X Ray Scattering spectra. The combined use of computational and experimental methods enabled us to reduce experimental uncertainties in the determination of the true sample spectrum. Furthermore, the refined experimental spectrum of para-hydrogen and ortho-deuterium is consistently reproduced by both FK-LPI and RPMD results at momentum transfers lower than 12.8 nm(-1). At larger momentum transfers the FK-LPI results agree with experiment much better for ortho-deuterium than for para-hydrogen. More specifically we found that for k ∼ 20.0 nm(-1) para-hydrogen provides a test case for improved approximations to quantum dynamics.

High-resolution reversible folding of hyperstable RNA tetraloops using molecular dynamics simulations

PubMed Central

Chen, Alan A.; García, Angel E.

2013-01-01

We report the de novo folding of three hyperstable RNA tetraloops to 1–3 Å rmsd from their experimentally determined structures using molecular dynamics simulations initialized in the unfolded state. RNA tetraloops with loop sequences UUCG, GCAA, or CUUG are hyperstable because of the formation of noncanonical loop-stabilizing interactions, and they are all faithfully reproduced to angstrom-level accuracy in replica exchange molecular dynamics simulations, including explicit solvent and ion molecules. This accuracy is accomplished using unique RNA parameters, in which biases that favor rigid, highly stacked conformations are corrected to accurately capture the inherent flexibility of ssRNA loops, accurate base stacking energetics, and purine syn-anti interconversions. In a departure from traditional quantum chemistrycentric approaches to force field optimization, our parameters are calibrated directly from thermodynamic and kinetic measurements of intra- and internucleotide structural transitions. The ability to recapitulate the signature noncanonical interactions of the three most abundant hyperstable stem loop motifs represents a significant milestone to the accurate prediction of RNA tertiary structure using unbiased all-atom molecular dynamics simulations. PMID:24043821

Development of massive multilevel molecular dynamics simulation program, Platypus (PLATform for dYnamic Protein Unified Simulation), for the elucidation of protein functions.

PubMed

Takano, Yu; Nakata, Kazuto; Yonezawa, Yasushige; Nakamura, Haruki

2016-05-05

A massively parallel program for quantum mechanical-molecular mechanical (QM/MM) molecular dynamics simulation, called Platypus (PLATform for dYnamic Protein Unified Simulation), was developed to elucidate protein functions. The speedup and the parallelization ratio of Platypus in the QM and QM/MM calculations were assessed for a bacteriochlorophyll dimer in the photosynthetic reaction center (DIMER) on the K computer, a massively parallel computer achieving 10 PetaFLOPs with 705,024 cores. Platypus exhibited the increase in speedup up to 20,000 core processors at the HF/cc-pVDZ and B3LYP/cc-pVDZ, and up to 10,000 core processors by the CASCI(16,16)/6-31G** calculations. We also performed excited QM/MM-MD simulations on the chromophore of Sirius (SIRIUS) in water. Sirius is a pH-insensitive and photo-stable ultramarine fluorescent protein. Platypus accelerated on-the-fly excited-state QM/MM-MD simulations for SIRIUS in water, using over 4000 core processors. In addition, it also succeeded in 50-ps (200,000-step) on-the-fly excited-state QM/MM-MD simulations for the SIRIUS in water. © 2016 The Authors. Journal of Computational Chemistry Published by Wiley Periodicals, Inc.

Large-Scale First-Principles Molecular Dynamics Simulations with Electrostatic Embedding: Application to Acetylcholinesterase Catalysis

DOE PAGES

Fattebert, Jean-Luc; Lau, Edmond Y.; Bennion, Brian J.; ...

2015-10-22

Enzymes are complicated solvated systems that typically require many atoms to simulate their function with any degree of accuracy. We have recently developed numerical techniques for large scale First-Principles molecular dynamics simulations and applied them to study the enzymatic reaction catalyzed by acetylcholinesterase. We carried out Density functional theory calculations for a quantum mechanical (QM) sub- system consisting of 612 atoms with an O(N) complexity finite-difference approach. The QM sub-system is embedded inside an external potential field representing the electrostatic effect due to the environment. We obtained finite temperature sampling by First-Principles molecular dynamics for the acylation reaction of acetylcholinemore » catalyzed by acetylcholinesterase. Our calculations shows two energies barriers along the reaction coordinate for the enzyme catalyzed acylation of acetylcholine. In conclusion, the second barrier (8.5 kcal/mole) is rate-limiting for the acylation reaction and in good agreement with experiment.« less

Quantum analogue computing.

PubMed

Kendon, Vivien M; Nemoto, Kae; Munro, William J

2010-08-13

We briefly review what a quantum computer is, what it promises to do for us and why it is so hard to build one. Among the first applications anticipated to bear fruit is the quantum simulation of quantum systems. While most quantum computation is an extension of classical digital computation, quantum simulation differs fundamentally in how the data are encoded in the quantum computer. To perform a quantum simulation, the Hilbert space of the system to be simulated is mapped directly onto the Hilbert space of the (logical) qubits in the quantum computer. This type of direct correspondence is how data are encoded in a classical analogue computer. There is no binary encoding, and increasing precision becomes exponentially costly: an extra bit of precision doubles the size of the computer. This has important consequences for both the precision and error-correction requirements of quantum simulation, and significant open questions remain about its practicality. It also means that the quantum version of analogue computers, continuous-variable quantum computers, becomes an equally efficient architecture for quantum simulation. Lessons from past use of classical analogue computers can help us to build better quantum simulators in future.

Floquet–Magnus theory and generic transient dynamics in periodically driven many-body quantum systems

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

Kuwahara, Tomotaka, E-mail: tomotaka.phys@gmail.com; WPI, Advanced Institute for Materials Research, Tohoku University, Sendai 980-8577; Mori, Takashi

2016-04-15

This work explores a fundamental dynamical structure for a wide range of many-body quantum systems under periodic driving. Generically, in the thermodynamic limit, such systems are known to heat up to infinite temperature states in the long-time limit irrespective of dynamical details, which kills all the specific properties of the system. In the present study, instead of considering infinitely long-time scale, we aim to provide a general framework to understand the long but finite time behavior, namely the transient dynamics. In our analysis, we focus on the Floquet–Magnus (FM) expansion that gives a formal expression of the effective Hamiltonian onmore » the system. Although in general the full series expansion is not convergent in the thermodynamics limit, we give a clear relationship between the FM expansion and the transient dynamics. More precisely, we rigorously show that a truncated version of the FM expansion accurately describes the exact dynamics for a certain time-scale. Our theory reveals an experimental time-scale for which non-trivial dynamical phenomena can be reliably observed. We discuss several dynamical phenomena, such as the effect of small integrability breaking, efficient numerical simulation of periodically driven systems, dynamical localization and thermalization. Especially on thermalization, we discuss a generic scenario on the prethermalization phenomenon in periodically driven systems. -- Highlights: •A general framework to describe transient dynamics for periodically driven systems. •The theory is applicable to generic quantum many-body systems including long-range interacting systems. •Physical meaning of the truncation of the Floquet–Magnus expansion is rigorously established. •New mechanism of the prethermalization is proposed. •Revealing an experimental time-scale for which non-trivial dynamical phenomena can be reliably observed.« less

Electronic coarse graining enhances the predictive power of molecular simulation allowing challenges in water physics to be addressed

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

Cipcigan, Flaviu S., E-mail: flaviu.cipcigan@ed.ac.uk; National Physical Laboratory, Hampton Road, Teddington, Middlesex TW11 0LW; Sokhan, Vlad P.

One key factor that limits the predictive power of molecular dynamics simulations is the accuracy and transferability of the input force field. Force fields are challenged by heterogeneous environments, where electronic responses give rise to biologically important forces such as many-body polarisation and dispersion. The importance of polarisation in the condensed phase was recognised early on, as described by Cochran in 1959 [Philosophical Magazine 4 (1959) 1082–1086] [32]. Currently in molecular simulation, dispersion forces are treated at the two-body level and in the dipole limit, although the importance of three-body terms in the condensed phase was demonstrated by Barker inmore » the 1980s [Phys. Rev. Lett. 57 (1986) 230–233] [72]. One approach for treating both polarisation and dispersion on an equal basis is to coarse grain the electrons surrounding a molecular moiety to a single quantum harmonic oscillator (cf. Hirschfelder, Curtiss and Bird 1954 [The Molecular Theory of Gases and Liquids (1954)] [37]). The approach, when solved in strong coupling beyond the dipole limit, gives a description of long-range forces that includes two- and many-body terms to all orders. In the last decade, the tools necessary to implement the strong coupling limit have been developed, culminating in a transferable model of water with excellent predictive power across the phase diagram. Transferability arises since the environment automatically identifies the important long range interactions, rather than the modeler through a limited set of expressions. Here, we discuss the role of electronic coarse-graining in predictive multiscale materials modelling and describe the first implementation of the method in a general purpose molecular dynamics software: QDO-MD. - Highlights: • Electronic coarse graining unites many-body dispersion and polarisation beyond the dipole limit. • It consists of replacing the electrons of a molecule using a quantum harmonic oscillator, called a Quantum Drude Oscillator. • We present the first general implementation of Quantum Drude Oscillators in the molecular dynamics package QDO-MD. • We highlight the successful construction of a new, transferable molecular model of water: QDO-water. - Graphical abstract:.« less

QuTiP: An open-source Python framework for the dynamics of open quantum systems

NASA Astrophysics Data System (ADS)

Johansson, J. R.; Nation, P. D.; Nori, Franco

2012-08-01

We present an object-oriented open-source framework for solving the dynamics of open quantum systems written in Python. Arbitrary Hamiltonians, including time-dependent systems, may be built up from operators and states defined by a quantum object class, and then passed on to a choice of master equation or Monte Carlo solvers. We give an overview of the basic structure for the framework before detailing the numerical simulation of open system dynamics. Several examples are given to illustrate the build up to a complete calculation. Finally, we measure the performance of our library against that of current implementations. The framework described here is particularly well suited to the fields of quantum optics, superconducting circuit devices, nanomechanics, and trapped ions, while also being ideal for use in classroom instruction. Catalogue identifier: AEMB_v1_0 Program summary URL:http://cpc.cs.qub.ac.uk/summaries/AEMB_v1_0.html Program obtainable from: CPC Program Library, Queen's University, Belfast, N. Ireland Licensing provisions: GNU General Public License, version 3 No. of lines in distributed program, including test data, etc.: 16 482 No. of bytes in distributed program, including test data, etc.: 213 438 Distribution format: tar.gz Programming language: Python Computer: i386, x86-64 Operating system: Linux, Mac OSX, Windows RAM: 2+ Gigabytes Classification: 7 External routines: NumPy (http://numpy.scipy.org/), SciPy (http://www.scipy.org/), Matplotlib (http://matplotlib.sourceforge.net/) Nature of problem: Dynamics of open quantum systems. Solution method: Numerical solutions to Lindblad master equation or Monte Carlo wave function method. Restrictions: Problems must meet the criteria for using the master equation in Lindblad form. Running time: A few seconds up to several tens of minutes, depending on size of underlying Hilbert space.

Coherent feedback control of a single qubit in diamond

NASA Astrophysics Data System (ADS)

Hirose, Masashi; Cappellaro, Paola

2016-04-01

Engineering desired operations on qubits subjected to the deleterious effects of their environment is a critical task in quantum information processing, quantum simulation and sensing. The most common approach relies on open-loop quantum control techniques, including optimal-control algorithms based on analytical or numerical solutions, Lyapunov design and Hamiltonian engineering. An alternative strategy, inspired by the success of classical control, is feedback control. Because of the complications introduced by quantum measurement, closed-loop control is less pervasive in the quantum setting and, with exceptions, its experimental implementations have been mainly limited to quantum optics experiments. Here we implement a feedback-control algorithm using a solid-state spin qubit system associated with the nitrogen vacancy centre in diamond, using coherent feedback to overcome the limitations of measurement-based feedback, and show that it can protect the qubit against intrinsic dephasing noise for milliseconds. In coherent feedback, the quantum system is connected to an auxiliary quantum controller (ancilla) that acquires information about the output state of the system (by an entangling operation) and performs an appropriate feedback action (by a conditional gate). In contrast to open-loop dynamical decoupling techniques, feedback control can protect the qubit even against Markovian noise and for an arbitrary period of time (limited only by the coherence time of the ancilla), while allowing gate operations. It is thus more closely related to quantum error-correction schemes, although these require larger and increasing qubit overheads. Increasing the number of fresh ancillas enables protection beyond their coherence time. We further evaluate the robustness of the feedback protocol, which could be applied to quantum computation and sensing, by exploring a trade-off between information gain and decoherence protection, as measurement of the ancilla-qubit correlation after the feedback algorithm voids the protection, even if the rest of the dynamics is unchanged.

Computational quantum-classical boundary of noisy commuting quantum circuits

PubMed Central

Fujii, Keisuke; Tamate, Shuhei

2016-01-01

It is often said that the transition from quantum to classical worlds is caused by decoherence originated from an interaction between a system of interest and its surrounding environment. Here we establish a computational quantum-classical boundary from the viewpoint of classical simulatability of a quantum system under decoherence. Specifically, we consider commuting quantum circuits being subject to decoherence. Or equivalently, we can regard them as measurement-based quantum computation on decohered weighted graph states. To show intractability of classical simulation in the quantum side, we utilize the postselection argument and crucially strengthen it by taking noise effect into account. Classical simulatability in the classical side is also shown constructively by using both separable criteria in a projected-entangled-pair-state picture and the Gottesman-Knill theorem for mixed state Clifford circuits. We found that when each qubit is subject to a single-qubit complete-positive-trace-preserving noise, the computational quantum-classical boundary is sharply given by the noise rate required for the distillability of a magic state. The obtained quantum-classical boundary of noisy quantum dynamics reveals a complexity landscape of controlled quantum systems. This paves a way to an experimentally feasible verification of quantum mechanics in a high complexity limit beyond classically simulatable region. PMID:27189039

Computational quantum-classical boundary of noisy commuting quantum circuits.

PubMed

Fujii, Keisuke; Tamate, Shuhei

2016-05-18

It is often said that the transition from quantum to classical worlds is caused by decoherence originated from an interaction between a system of interest and its surrounding environment. Here we establish a computational quantum-classical boundary from the viewpoint of classical simulatability of a quantum system under decoherence. Specifically, we consider commuting quantum circuits being subject to decoherence. Or equivalently, we can regard them as measurement-based quantum computation on decohered weighted graph states. To show intractability of classical simulation in the quantum side, we utilize the postselection argument and crucially strengthen it by taking noise effect into account. Classical simulatability in the classical side is also shown constructively by using both separable criteria in a projected-entangled-pair-state picture and the Gottesman-Knill theorem for mixed state Clifford circuits. We found that when each qubit is subject to a single-qubit complete-positive-trace-preserving noise, the computational quantum-classical boundary is sharply given by the noise rate required for the distillability of a magic state. The obtained quantum-classical boundary of noisy quantum dynamics reveals a complexity landscape of controlled quantum systems. This paves a way to an experimentally feasible verification of quantum mechanics in a high complexity limit beyond classically simulatable region.

Computational quantum-classical boundary of noisy commuting quantum circuits

NASA Astrophysics Data System (ADS)

Fujii, Keisuke; Tamate, Shuhei

2016-05-01

It is often said that the transition from quantum to classical worlds is caused by decoherence originated from an interaction between a system of interest and its surrounding environment. Here we establish a computational quantum-classical boundary from the viewpoint of classical simulatability of a quantum system under decoherence. Specifically, we consider commuting quantum circuits being subject to decoherence. Or equivalently, we can regard them as measurement-based quantum computation on decohered weighted graph states. To show intractability of classical simulation in the quantum side, we utilize the postselection argument and crucially strengthen it by taking noise effect into account. Classical simulatability in the classical side is also shown constructively by using both separable criteria in a projected-entangled-pair-state picture and the Gottesman-Knill theorem for mixed state Clifford circuits. We found that when each qubit is subject to a single-qubit complete-positive-trace-preserving noise, the computational quantum-classical boundary is sharply given by the noise rate required for the distillability of a magic state. The obtained quantum-classical boundary of noisy quantum dynamics reveals a complexity landscape of controlled quantum systems. This paves a way to an experimentally feasible verification of quantum mechanics in a high complexity limit beyond classically simulatable region.

Quantum Monte Carlo study of the transverse-field quantum Ising model on infinite-dimensional structures

NASA Astrophysics Data System (ADS)

Baek, Seung Ki; Um, Jaegon; Yi, Su Do; Kim, Beom Jun

2011-11-01

In a number of classical statistical-physical models, there exists a characteristic dimensionality called the upper critical dimension above which one observes the mean-field critical behavior. Instead of constructing high-dimensional lattices, however, one can also consider infinite-dimensional structures, and the question is whether this mean-field character extends to quantum-mechanical cases as well. We therefore investigate the transverse-field quantum Ising model on the globally coupled network and on the Watts-Strogatz small-world network by means of quantum Monte Carlo simulations and the finite-size scaling analysis. We confirm that both of the structures exhibit critical behavior consistent with the mean-field description. In particular, we show that the existing cumulant method has difficulty in estimating the correct dynamic critical exponent and suggest that an order parameter based on the quantum-mechanical expectation value can be a practically useful numerical observable to determine critical behavior when there is no well-defined dimensionality.

Phonon impact on optical control schemes of quantum dots: Role of quantum dot geometry and symmetry

NASA Astrophysics Data System (ADS)

Lüker, S.; Kuhn, T.; Reiter, D. E.

2017-12-01

Phonons strongly influence the optical control of semiconductor quantum dots. When modeling the electron-phonon interaction in several theoretical approaches, the quantum dot geometry is approximated by a spherical structure, though typical self-assembled quantum dots are strongly lens-shaped. By explicitly comparing simulations of a spherical and a lens-shaped dot using a well-established correlation expansion approach, we show that, indeed, lens-shaped dots can be exactly mapped to a spherical geometry when studying the phonon influence on the electronic system. We also give a recipe to reproduce spectral densities from more involved dots by rather simple spherical models. On the other hand, breaking the spherical symmetry has a pronounced impact on the spatiotemporal properties of the phonon dynamics. As an example we show that for a lens-shaped quantum dot, the phonon emission is strongly concentrated along the direction of the smallest axis of the dot, which is important for the use of phonons for the communication between different dots.

Trapped atomic ions for quantum-limited metrology

NASA Astrophysics Data System (ADS)

Wineland, David

2017-04-01

Laser-beam-manipulated trapped ions are a candidate for large-scale quantum information processing and quantum simulation but the basic techniques used can also be applied to quantum-limited metrology and sensing. Some examples being explored at NIST are: 1) As charged harmonic oscillators, trapped ions can be used to sense electric fields; this can be used to characterize the electrode-surface-based noisy electric fields that compromise logic-gate fidelities and may eventually be used as a tool in surface science. 2) Since typical qubit logic gates depend on state-dependent forces, we can adapt the gate dynamics to sensitively detect additional forces. 3) We can use extensions of Bell inequality measurements to further restrict the degree of local realism possessed by Bell states. 4) We also briefly describe experiments for creation of Bell states using Hilbert space engineering. This work is a joint effort including the Ion-Storage group, the Quantum processing group, and the Computing and Communications Theory group at NIST, Boulder. Supported by IARPA, ONR, and the NIST Quantum Information Program.

Fluctuating hydrodynamics, current fluctuations, and hyperuniformity in boundary-driven open quantum chains

NASA Astrophysics Data System (ADS)

Carollo, Federico; Garrahan, Juan P.; Lesanovsky, Igor; Pérez-Espigares, Carlos

2017-11-01

We consider a class of either fermionic or bosonic noninteracting open quantum chains driven by dissipative interactions at the boundaries and study the interplay of coherent transport and dissipative processes, such as bulk dephasing and diffusion. Starting from the microscopic formulation, we show that the dynamics on large scales can be described in terms of fluctuating hydrodynamics. This is an important simplification as it allows us to apply the methods of macroscopic fluctuation theory to compute the large deviation (LD) statistics of time-integrated currents. In particular, this permits us to show that fermionic open chains display a third-order dynamical phase transition in LD functions. We show that this transition is manifested in a singular change in the structure of trajectories: while typical trajectories are diffusive, rare trajectories associated with atypical currents are ballistic and hyperuniform in their spatial structure. We confirm these results by numerically simulating ensembles of rare trajectories via the cloning method, and by exact numerical diagonalization of the microscopic quantum generator.

Fluctuating hydrodynamics, current fluctuations, and hyperuniformity in boundary-driven open quantum chains.

PubMed

Carollo, Federico; Garrahan, Juan P; Lesanovsky, Igor; Pérez-Espigares, Carlos

2017-11-01

We consider a class of either fermionic or bosonic noninteracting open quantum chains driven by dissipative interactions at the boundaries and study the interplay of coherent transport and dissipative processes, such as bulk dephasing and diffusion. Starting from the microscopic formulation, we show that the dynamics on large scales can be described in terms of fluctuating hydrodynamics. This is an important simplification as it allows us to apply the methods of macroscopic fluctuation theory to compute the large deviation (LD) statistics of time-integrated currents. In particular, this permits us to show that fermionic open chains display a third-order dynamical phase transition in LD functions. We show that this transition is manifested in a singular change in the structure of trajectories: while typical trajectories are diffusive, rare trajectories associated with atypical currents are ballistic and hyperuniform in their spatial structure. We confirm these results by numerically simulating ensembles of rare trajectories via the cloning method, and by exact numerical diagonalization of the microscopic quantum generator.

Constructing polyatomic potential energy surfaces by interpolating diabatic Hamiltonian matrices with demonstration on green fluorescent protein chromophore

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

Park, Jae Woo; Rhee, Young Min, E-mail: ymrhee@postech.ac.kr; Department of Chemistry, Pohang University of Science and Technology

2014-04-28

Simulating molecular dynamics directly on quantum chemically obtained potential energy surfaces is generally time consuming. The cost becomes overwhelming especially when excited state dynamics is aimed with multiple electronic states. The interpolated potential has been suggested as a remedy for the cost issue in various simulation settings ranging from fast gas phase reactions of small molecules to relatively slow condensed phase dynamics with complex surrounding. Here, we present a scheme for interpolating multiple electronic surfaces of a relatively large molecule, with an intention of applying it to studying nonadiabatic behaviors. The scheme starts with adiabatic potential information and its diabaticmore » transformation, both of which can be readily obtained, in principle, with quantum chemical calculations. The adiabatic energies and their derivatives on each interpolation center are combined with the derivative coupling vectors to generate the corresponding diabatic Hamiltonian and its derivatives, and they are subsequently adopted in producing a globally defined diabatic Hamiltonian function. As a demonstration, we employ the scheme to build an interpolated Hamiltonian of a relatively large chromophore, para-hydroxybenzylidene imidazolinone, in reference to its all-atom analytical surface model. We show that the interpolation is indeed reliable enough to reproduce important features of the reference surface model, such as its adiabatic energies and derivative couplings. In addition, nonadiabatic surface hopping simulations with interpolation yield population transfer dynamics that is well in accord with the result generated with the reference analytic surface. With these, we conclude by suggesting that the interpolation of diabatic Hamiltonians will be applicable for studying nonadiabatic behaviors of sizeable molecules.« less

Lattice constants of pure methane and carbon dioxide hydrates at low temperatures. Implementing quantum corrections to classical molecular dynamics studies

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

Costandy, Joseph; Michalis, Vasileios K.; Economou, Ioannis G., E-mail: i.tsimpanogiannis@qatar.tamu.edu, E-mail: ioannis.economou@qatar.tamu.edu

2016-03-28

We introduce a simple correction to the calculation of the lattice constants of fully occupied structure sI methane or carbon dioxide pure hydrates that are obtained from classical molecular dynamics simulations using the TIP4PQ/2005 water force field. The obtained corrected lattice constants are subsequently used in order to obtain isobaric thermal expansion coefficients of the pure gas hydrates that exhibit a trend that is significantly closer to the experimental behavior than previously reported classical molecular dynamics studies.