Journal ArticleDOI
Multilayer formulation of the multiconfiguration time-dependent Hartree theory
Haobin Wang,Michael Thoss +1 more
TLDR
In this paper, a multilayer formulation of the multiconfiguration time-dependent Hartree (MCTDH) theory is presented, where the single-particle (SP) functions in the original MCTDH method are further expressed employing a timedependent multi-figurational expansion, and the Dirac-Frenkel variational principle is applied to optimally determine the equations of motion.Abstract:
A multilayer (ML) formulation of the multiconfiguration time-dependent Hartree (MCTDH) theory is presented. In this new approach, the single-particle (SP) functions in the original MCTDH method are further expressed employing a time-dependent multiconfigurational expansion. The Dirac–Frenkel variational principle is then applied to optimally determine the equations of motion. Following this strategy, the SP groups are built in several layers, where each top layer SP can contain many more Cartesian degrees of freedom than in the previous formulation of the MCTDH method. As a result, the ML-MCTDH method has the capability of treating substantially more physical degrees of freedom than the original MCTDH method, and thus significantly enhances the ability of carrying out quantum dynamical simulations for complex molecular systems. The efficiency of the new formulation is demonstrated by converged quantum dynamical simulations for systems with a few hundred to a thousand degrees of freedom.read more
Citations
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Journal ArticleDOI
Influence of Coherent Tunneling and Incoherent Hopping on the Charge Transfer Mechanism in Linear Donor-Bridge-Acceptor Systems.
TL;DR: The quantum master equation (QME) approach is applied, based on second-order perturbation theory in a quantum dissipative system, to examine the dynamical processes involved in charge-transfer and follow the population transfer rate at the acceptor to shed light on the transition from tunneling to hopping.
Journal ArticleDOI
Collective excitations of dipolar gases based on local tunneling in superlattices
TL;DR: In this paper, the collective dynamics of a dipolar fermionic quantum gas confined in a one-dimensional double-well superlattice is explored, and a well-defined momentum-energy dispersion relation is identified in the ab-initio simulations demonstrating the phonon-like behavior.
Journal ArticleDOI
Low-frequency logarithmic discretization of the reservoir spectrum for improving the efficiency of hierarchical equations of motion approach.
TL;DR: The LFLD scheme requires a much smaller number of exponential functions than the conventional PSD scheme to reproduce the reservoir correlation function and thus facilitates the efficient implementation of the HEOM approach in extremely low temperature regimes.
Journal ArticleDOI
New coherent state representation for the imaginary time propagator with applications to forward-backward semiclassical initial value representations of correlation functions.
Eli Pollak,Eva Martin-Fierro +1 more
TL;DR: A similar but different expression is developed in which exp(-betaH) is represented in a series whose terms are weighted phase space averages of coherent states and allows for the formulation of a new and simplified forward-backward semiclassical initial value representation expression for thermal correlation functions.
Journal ArticleDOI
Full-dimensional quantum dynamics calculations for H + CHD3 → H2 + CD3: The effect of multiple vibrational excitations.
Roman Ellerbrock,Uwe Manthe +1 more
TL;DR: It is found that energy deposited in overtones and combination bands is less efficient in promoting reactivity than expected from separable or sudden models.
References
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Light-Induced Redox Reactions in Nanocrystalline Systems
Anders Hagfeldt,Michael Graetzel +1 more
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TL;DR: In this article, a functional-integral approach to the dynamics of a two-state system coupled to a dissipative environment is presented, and an exact and general prescription for the reduction, under appropriate circumstances, of the problem of a system tunneling between two wells in the presence of dissipative environments to the spin-boson problem is given.
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Quantum Dissipative Systems
TL;DR: In this paper, the authors present a survey of the various approaches to Quantum-Statistical metastability, including Imaginary-Time and Real-Time Approaches Influence Functional Method Phenomenological and Microscopic System-Plus-Reservoir Models Linear and Nonlinear Quantum Environments Ohmic, Super-Ohmic, and Sub-ohmic Dissipation Quantum Decoherence and Relaxation Correlation Functions, Response Functions, and Fluctuation-Dissipation Theorem Damped Quantum Mechanical Harmonic Oscillator Quantum Brownian Motion Thermodynamic Variational
Journal ArticleDOI
The multiconfiguration time-dependent Hartree (MCTDH) method: a highly efficient algorithm for propagating wavepackets
TL;DR: In this article, a review of the multiconfiguration time-dependent Hartree (MCTDH) method for propagating wavepackets is given, and the formal derivation, numerical implementation, and performance of the method are detailed.
Journal ArticleDOI
Trajectory Surface Hopping Approach to Nonadiabatic Molecular Collisions: The Reaction of H+ with D2
John C. Tully,Richard K. Preston +1 more
TL;DR: In this article, an extension of the classical trajectory approach is proposed that may be useful in treating many types of nonadiabatic molecular collisions, where nuclei are assumed to move classically on a single potential energy surface until an avoided surface crossing or other region of large NDE coupling is reached.