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
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Spin-Vibronic Mechanism for Intersystem Crossing
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References
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Semiclassical theory of electronically nonadiabatic dynamics: results of a linearized approximation to the initial value representation
TL;DR: In this paper, a linearized approximation to the semiclassical initial value representation (SC-IVR) was used to calculate reactive flux correlation functions for a model of a chemical reaction on a single potential energy surface.
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Time‐dependent self‐consistent field approximation for intramolecular energy transfer. I. Formulation and application to dissociation of van der Waals molecules
TL;DR: The time-dependent self-consistent field method (TDSCF) as mentioned in this paper has been applied to the study of intramolecular dynamics and unimolecular decomposition processes.
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Spiers Memorial Lecture Quantum and semiclassical theory of chemical reaction rates
TL;DR: In this paper, the semiclassical (SC) initial value representation (IVR) is applied to models of unimolecular isomerization and electronic non-adiabatic transitions coupled to an infinite bath of harmonic oscillators.
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The Role of Surface States in the Ultrafast Photoinduced Electron Transfer from Sensitizing Dye Molecules to Semiconductor Colloids
TL;DR: In this article, the authors investigated the ultrafast electron injection mechanism from the dye alizarin to wide band gap semiconductor colloids in aqueous medium, combined with detailed studies on population, depopulation, and relaxation phenomena in trap states and their influence on the injection process.
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Self-consistent hybrid approach for complex systems: Application to the spin-boson model with Debye spectral density
TL;DR: In this paper, Wang et al. applied the self-consistent hybrid approach to the spin-boson problem with Debye spectral density as a model for electron-transfer reactions in a solvent exhibiting Debye dielectric relaxation.