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
Semiclassical analysis of the electron-nuclear coupling in electronic non-adiabatic processes
TL;DR: In this paper, the authors describe a numerical procedure to approximate the electron-nuclear coupling operator within a semiclassical treatment of the nuclear dynamics, with the aim of describing the properties of the operator.
Journal ArticleDOI
Mixed quantum-classical electrodynamics: Understanding spontaneous decay and zero-point energy
Tao E. Li,Abraham Nitzan,Maxim Sukharev,Todd J. Martínez,Todd J. Martínez,Hsing-Ta Chen,Joseph E. Subotnik +6 more
TL;DR: In this article, the authors consider three flavors of mixed quantum-classical dynamics: (i) the classical path approximation, (ii) Ehrenfest dynamics, and (iii) symmetrical quasiclassical (SQC) dynamics.
Journal ArticleDOI
Multimode quantum dynamics with multiple Davydov D2 trial states: Application to a 24-dimensional conical intersection model.
TL;DR: The ultrafast nonadiabatic dynamics of a two-electronic-state four-vibrational-mode conical intersection coupled to a finite bath with up to 20 harmonic oscillators has been investigated by employing the multiple Davydov D2 ansatz.
Journal ArticleDOI
Intramolecular Singlet Fission: Insights from Quantum Dynamical Simulations.
TL;DR: The results show that the population of the multiexcitonic state, corresponding to the first step of singlet fission, is facilitated by the existence of higher-lying doubly excited and charge transfer states that participate in a superexchange-like way.
Journal ArticleDOI
A full-dimensional multilayer multiconfiguration time-dependent Hartree study on the ultraviolet absorption spectrum of formaldehyde oxide.
Qingyong Meng,Hans-Dieter Meyer +1 more
TL;DR: This is the first theoretical UV spectrum simulated for this molecule including nuclear motion beyond an adiabatic harmonic approximation, and even for the present not-too-large system (9D here) the ML-MCTDH calculations can save a considerable amount of computational resources while producing identical spectra as the MCT DH calculations.
References
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Light-Induced Redox Reactions in Nanocrystalline Systems
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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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