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
Quantum dynamics and spectroscopy of dihalogens in solid matrices. I. Efficient simulation of the photodynamics of the embedded $\mathrm{I_2 Kr_{18}}$ cluster using the G-MCTDH method
TL;DR: In this article, a Gaussian variant of the multiconfigurational time-dependent Hartree method (G-MCTDH) was used to simulate the photoexcitation of the iodine molecule embedded in solid krypton.
Journal ArticleDOI
Using n-mode potentials for reactive scattering: Application to the 6D H 2 + Pt(1 1 1) problem
TL;DR: In this paper, the accuracy of n-mode representations of potential energy surfaces (PESs) is investigated, for a reaction involving six degrees of freedom, and the results suggest that n -mode representations can be employed successfully to study reactions of polyatomic molecules with surfaces.
Journal ArticleDOI
On the accuracy of the noninteracting electron approximation for vibrationally coupled electron transport
Haobin Wang,Michael Thoss +1 more
TL;DR: In this article, the accuracy of the noninteracting electron approximation for a model of vibrationally coupled electron transport in single molecule junction is examined for the absence of electronic-vibrational coupling, steady state transport in this model is described exactly by Landauer theory.
Journal ArticleDOI
Quantum dynamical simulation of intramolecular singlet fission in covalently coupled pentacene dimers
TL;DR: The results highlight the different role of the direct and mediated mechanism in these systems, showing that the population of the multiexcitonic state, corresponding to the first step of the intramolecular singlet fission process, occurs mainly through a superexchange-like mechanism involving doubly excited or charge transfer states that participate in the process in a virtual way.
Journal ArticleDOI
Performance evaluation of the symmetrical quasi-classical dynamics method based on Meyer-Miller mapping Hamiltonian in the treatment of site-exciton models
TL;DR: In this paper, the authors evaluated the performance of the MM-SQC method in various site-exciton models with respect to the accurate results of quantum dynamics method multilayer multiconfigurational time-dependent Hartree (ML-MCTDH).
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.
Journal ArticleDOI
Trajectory Surface Hopping Approach to Nonadiabatic Molecular Collisions: The Reaction of H+ with D2
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