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
Ultrafast Dynamics of the Two Lowest Bright Excited States of Cytosine and 1-Methylcytosine: A Quantum Dynamical Study.
TL;DR: To run QD simulations of cytosine and 1-methyl-cytosine in gas phase, an automatic general procedure to parametrize linear vibronic coupling models with time-dependent density functional theory (DFT) computations was implemented, and the wavepacket was propagated with the multilayer version of the multiconfigurational time dependent Hartree method.
Journal ArticleDOI
Dynamical pruning of the multiconfiguration time-dependent Hartree (DP-MCTDH) method: An efficient approach for multidimensional quantum dynamics.
Henrik Larsson,David J. Tannor +1 more
TL;DR: Two strategies for combining dynamical pruning with the multiconfiguration time-dependent Hartree (DP-MCTDH) method are presented, where dynamicalPruning means on-the-fly selection of relevant basis functions.
Journal ArticleDOI
Efficient molecular quantum dynamics in coordinate and phase space using pruned bases
TL;DR: This work combines the ideas behind the biorthogonal von Neumann basis (PvB) with the orthogonalized momentum-symmetrized Gaussians (Weylets) to create a new basis, projected Weylets, that takes the best from both methods.
Journal ArticleDOI
Topologically Correct Quantum Nonadiabatic Formalism for On-the-Fly Dynamics.
TL;DR: In this paper, the authors analyze two approaches for nonadiabatic dynamics using the time-dependent variational principle and the adiabatic representation, and show that unless a gauge transformation is used to enforce single-valued boundary conditions, the first approach fails to capture the geometric phase.
Journal ArticleDOI
Dynamics of a two-level system coupled to a bath of spins.
Haobin Wang,Jiushu Shao +1 more
TL;DR: It is found that increasing temperature favors quantum coherence in the nonadiabatic limit of this model, which corroborates the prediction in the previous work based on the non-interacting blip approximation (NIBA).
References
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Journal ArticleDOI
Light-Induced Redox Reactions in Nanocrystalline Systems
Anders Hagfeldt,Michael Graetzel +1 more
TL;DR: A review with 156 refs on interfacial electron transfer reactions in colloidal semiconductor solns and thin films and their application for solar light energy conversion and photocatalytic water purifn is presented in this paper.
Journal ArticleDOI
Dynamics of the dissipative two-state system
Anthony J. Leggett,Sudip Chakravarty,Alan T. Dorsey,Matthew P. A. Fisher,Anupam Garg,Wilhelm Zwerger +5 more
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.
Book
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.