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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Non-Markovian stochastic Schrödinger equation: Matrix-product-state approach to the hierarchy of pure states
TL;DR: In this paper , a stochastic hierarchy of matrix product states (HOMPS) is derived for non-Markovian dynamics in open quantum system at finite temperature, which is numerically exact and efficient.
Journal ArticleDOI
A reciprocal-space formulation of mixed quantum-classical dynamics.
TL;DR: In this article, the authors derived a mixed quantum-classical dynamics for modeling electronic carriers interacting with phonons in reciprocal space, which is equivalent to mean-field mixed quantum classical dynamics in real space.
Time Evolution in Open Quantum Systems - From Exciton Dynamics to Charge Transport
TL;DR: In this paper, three main formalisms that are presented in this work include quantum master equations (QME), in second order perturbation theory in the system-reservoir coupling, the hierarchical equations of motion (HEOM) scheme for multi-particle bosonic systems as well as a scheme based on time-dependent nonequilibrium Green's functions (NEGF) for non-interacting fermionic systems.
Journal ArticleDOI
High-Dimensional Quantum Dynamics Study on Excitation-Specific Surface Scattering Including Lattice Effects of a Five-Atom Surface Cell.
TL;DR: High-dimensional (21D) quantum dynamics calculations on the mode-specific surface scattering of a carbon monoxide molecule on a copper(100) surface with lattice effects of a five-atom surface cell are performed through the multilayer multiconfiguration time-dependent Hartree (ML-MCTDH) method.
Journal ArticleDOI
Modeling Non-Reversible Molecular Internal Conversion Using the Time-dependent Variational Approach with sD2 Ansatz
TL;DR: In this paper, the effects of non-linear coupling between the system and the bath vibrational modes on the system internal conversion dynamics are investigated using the Dirac-Frenkel variational approach with the defined sD2 ansatz.
References
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Light-Induced Redox Reactions in Nanocrystalline Systems
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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
John C. Tully,Richard K. Preston +1 more
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