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
Journal ArticleDOI
Semiquantal molecular dynamics simulations of hydrogen-bond dynamics in liquid water using multi-dimensional Gaussian wave packets.
Junichi Ono,Koji Ando +1 more
TL;DR: It is found that the anisotropy of the WPs is indispensable for reproducing the disordered H-bond network compared to the classical counterpart with the use of the potential model providing competing quantum effects between intra- and intermolecular zero-point fluctuations.
Journal ArticleDOI
On-the-Fly Symmetrical Quasi-Classical Dynamics with Meyer-Miller Mapping Hamiltonian for the Treatment of Nonadiabatic Dynamics at Conical Intersections.
TL;DR: In this paper, the on-the-fly version of the symmetrical quasi-classical dynamics method based on the Meyer-Miller mapping Hamiltonian (SQC/MM) is implemented to study the nonadiabatic dynamics at conical intersections of polyatomic systems.
Journal ArticleDOI
The multi-configurational time-dependent Hartree approach in optimized second quantization: Imaginary time propagation and particle number conservation.
Thomas Weike,Uwe Manthe +1 more
TL;DR: The multilayer multiconfigurational time-dependent Hartree (MCTDH) in optimized second quantization representation (oSQR) approach combines the tensor contraction scheme of the multilayers MCTDH approach with the use of an optimized time- dependent orbital basis.
Journal ArticleDOI
Modeling Intermolecular and Intramolecular Modes of Liquid Water Using Multiple Heat Baths: Machine Learning Approach
Seiji Ueno,Yoshitaka Tanimura +1 more
TL;DR: A system-bath model is introduced in which the intramolecular modes with anharmonic mode-mode couplings are described by a system Hamiltonian, while the other degrees of freedom, arising from the environmental molecules, are describing by heat bath.
Journal ArticleDOI
Quantum Dynamics Simulations of Excited State Energy Transfer in a Zinc-Free-Base Porphyrin Dyad.
TL;DR: To successfully simulate the EET process, it is important to include coupling between nuclear and electronic degrees of freedom in the QD simulation, account for Coulomb coupling between the electron and hole wavepackets, and parametrize the extended Hückel model Hamiltonian employed in theQD simulations with respect to the DFT.
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.