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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Hermite-distributed approximating functional-based formulation of multiconfiguration time-dependent Hartree method: A case study of quantum tunnelling in a coupled double-well system
TL;DR: In this article, the authors proposed a variant of the multiconfiguration time-dependent Hartree (MCTDH) method within the framework of Hermite-distributed approximating functional (HDAF) method for tunnelling dynamics of two coupled double well oscillators.
Journal ArticleDOI
Quantum dynamics of relaxation of a pair of coupled morse oscillators : Effects of mass and electrical asymmetries
TL;DR: In this paper, a multiconfiguration time-dependent Hartree method based recipe is used to study the role of mass and electrical asymmetry in controlling the quantum dynamics of relaxation of a locally excited O-H bond in a water molecule, modeled by a pair of interacting Morse oscillators.
QD3SET-1: A Database with Quantum Dissipative Dynamics Data Sets
TL;DR: In this article , the authors present a new database QD3SET-1 containing eight data sets of quantum dynamical data for two systems of broad interest, spin-boson (SB) model and the Fenna-Matthews-Olson (FMO) complex, generated with two different methods solving the dynamics, approximate local thermalizing Lindblad master equation (LTLME) and highly accurate hierarchy equations of motion (HEOM).
Journal ArticleDOI
Quantendynamik offener Systeme, Trendbericht Theoretische Chemie 2020, Teil 3
TL;DR: In this paper, the authors provide an overview of recent numerical methods suited to describe the nonperturbative regime of system bath interaction and provide a rigorous description of the process of decoherence.
Journal ArticleDOI
Quantum Dynamics Simulation of Doublet Excitation and Magnetic Field Effect in Neutral Radical Materials.
TL;DR: The photon absorption and the relevant magnetic field effect of a doublet in neutral radical materials are investigated by combining the density functional theory and the variational quantum dynamics with Davydov ansatz, leading to a result which can be described by a sum of Lorentzian functions.
References
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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
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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.
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Trajectory Surface Hopping Approach to Nonadiabatic Molecular Collisions: The Reaction of H+ with D2
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