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
More filters
Posted ContentDOI
Multiphoton Excitation of Organic Molecules in a Cavity – Superradiance as a Measure of Coherence
TL;DR: In this paper, wave packet propagations for various pyrazine models of increasing complexity and molecular ensembles thereof were studied and it was shown that ensemble coherence upon photoexcitation can prevail up to relatively long time scales, although the effect can diminish quickly with increasing ensemble size.
Journal ArticleDOI
A Structure-Based Gaussian Expansion for Quantum Reaction Dynamics in Molecules: Application to Hydrogen Tunneling in Malonaldehyde.
TL;DR: In this paper , a structure-based Gaussian (SBG) expansion approach is proposed for quantum reaction dynamics simulations, where SBG bases for the expansion of the wave function are mainly placed around critical structures on reaction pathways such as on the intrinsic reaction coordinate (IRC) through a transition state.
Journal ArticleDOI
Reprint of “The effect of site-specific spectral densities on the high-dimensional exciton-vibrational dynamics in the FMO complex”
TL;DR: In this article, the effect of spectral density on the exciton state populations as well as on the vibrational and vibronic non-equilibrium excitations was investigated using the Multi-layer Multi-configuration Time-dependent Hartree (ML-MCTDH) approach.
Peer Review
Floquet nonadiabatic dynamics in open quantum systems
TL;DR: In this paper , the authors present the Floquet quantum master equation (FQCLE) and the mixed quantum classical Liouville equation (QCLE), which are general platforms for developing trajectory-based dynamical approaches.
Journal Article
Electron transfer in a two-level system within a Cole-Davidson vitreous bath
TL;DR: It is shown that at low temperatures and when the coupling to the bath is weak, the viscous bath preserves the quantum coherence for a longer time, however in the strong coupling regime, the tunneling rate is higher in the CD.
References
More filters
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.