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
Dynamical Approximation by Hierarchical Tucker and Tensor-Train Tensors
TL;DR: This approach can be used to approximate the solutions to tensor differential equations in the HT or TT format and to compute updates in optimization algorithms within these reduced tensor formats.
Journal ArticleDOI
Nonadiabatic Excited-State Molecular Dynamics Modeling of Photoinduced Dynamics in Conjugated Molecules
Tammie Nelson,Sebastian Fernandez-Alberti,Vladimir Y. Chernyak,Adrian E. Roitberg,Sergei Tretiak +4 more
TL;DR: This work has developed a nonadiabatic excited-state molecular dynamics (NA-ESMD) framework incorporating quantum transitions and identifies specific slow and fast nuclear motions that are strongly coupled to the electronic degrees of freedom, namely, torsion and bond length alternation.
Journal ArticleDOI
Multimode quantum dynamics using Gaussian wavepackets: The Gaussian-based multiconfiguration time-dependent Hartree (G-MCTDH) method applied to the absorption spectrum of pyrazine
TL;DR: The Gaussian-based multiconfiguration time-dependent Hartree (G-MCTDH) method is applied to calculate the S(2)(pipi( *)) absorption spectrum of the pyrazine molecule, whose diffuse structure results from the ultrafast nonadiabatic dynamics at the S (2)-S(1) conical intersection.
Journal ArticleDOI
Quantum Dynamics of Photoinduced Electron-Transfer Reactions in Dye−Semiconductor Systems: First-Principles Description and Application to Coumarin 343−TiO2
TL;DR: In this paper, a method to describe the quantum dynamics of photo-induced heterogeneous electron-transfer processes at dye−semiconductor interfaces is proposed, based on a model Hamiltonian, the parameters of which are determined by first-principles electronic structure calculations.
Journal ArticleDOI
Multilayer Multiconfiguration Time-Dependent Hartree Theory
TL;DR: The multilayer multiconfiguration time-dependent Hartree (ML-MCTDH) theory as mentioned in this paper is an extension of MCTDH to include dynamically contracted layers in a recursive way, within which the equations of motion are determined from the Dirac-Frenkel variational principle.
References
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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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