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
Multi-State Trajectory Approach to Non-Adiabatic Dynamics: General Formalism and the Active State Trajectory Approximation
TL;DR: In this paper, a general theoretical framework is derived for the recently developed multi-state trajectory (MST) approach from the time dependent Schrodinger equation, resulting in equations of motion for coupled nuclear-electronic dynamics equivalent to Hamilton dynamics or Heisenberg equation based on a new multistate Meyer-Miller (MM) model.
Journal ArticleDOI
First-Principles Theory for the Reaction of Chlorine with Methane.
Hans Hoppe,Uwe Manthe +1 more
TL;DR: In this paper , a full-dimensional quantum dynamics simulation of the Cl + CH4 → HCl + CH3 reaction based on first-principles theory is reported, and accurate thermal rate constants are calculated, and perfect agreement with experiment is obtained.
Book ChapterDOI
Quantum and Semiclassical Dynamics
TL;DR: In this article, the authors introduce quantum, semiclassical and mixed quantum-classical approaches for the study of the dynamics of chemical phenomena with a specific emphasis on photoinduced molecular processes occurring on coupled electronic states.
Journal ArticleDOI
Calculating vibrational excitation energies using tensor-decomposed vibrational coupled-cluster response theory.
TL;DR: The tensor-decomposed vibrational coupled cluster (CP-VCC) response theory for calculating vibrational excitation energies is presented in this article, which has previously been applied to solving the VCC ground-state equations without explicitly constructing any tensors of order three or higher.
Journal ArticleDOI
State-resolved infrared spectrum of the protonated water dimer: revisiting the characteristic proton transfer doublet peak
TL;DR: In this article , the interplay between the proton transfer and the water wagging motions in the Protonated Water dimer (Zundel ion) giving rise to the characteristic doublet peak is both more complex and more sensitive to subtle energetic changes than previously thought.
References
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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.
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Dynamics of the dissipative two-state system
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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.