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
Testing the multi-configuration time-dependent Hartree-Fock method
TL;DR: In this paper, the authors test the multi-configuration time-dependent Hartree-Fock method as a new approach towards numerical calculation of dynamical processes in multi-electron systems using the harmonic quantum dot and one-dimensional helium in strong laser pulses as models.
Journal ArticleDOI
An error analysis of the multi-configuration time-dependent Hartree method of quantum dynamics
Dajana Conte,Christian Lubich +1 more
TL;DR: In this article, an error analysis of the multi-configuration time-dependent Hartree (MCTDH) method for the approximation of multi-particle timedependent Schrodinger equations is given.
Journal ArticleDOI
Heat transport through model molecular junctions : A multilayer multiconfiguration time-dependent Hartree approach
TL;DR: In this article, a numerically exact approach is proposed to study heat transport through a molecular junction that is coupled to two phonon reservoirs at different temperatures within a spin-boson type model.
Journal ArticleDOI
Effect of the Anchoring Group on Electron Injection: Theoretical Study of Phosphonated Dyes for Dye-Sensitized Solar Cells
TL;DR: In this paper, the effect of the size and nature of the anchoring group on the injection times of a set of organic dyes on TiO2 rutile (110) and anatase (101) surfaces for the most stable adsorption geometries of the anchor group was analyzed.
Journal ArticleDOI
Ab initio quantum direct dynamics simulations of ultrafast photochemistry with Multiconfigurational Ehrenfest approach
TL;DR: The Multiconfigurational Ehrenfest (MCE) method as mentioned in this paper is a quantum dynamics technique which allows treatment of a large number of quantum nuclear degrees of freedom, and it has been applied in many applications.
References
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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
John C. Tully,Richard K. Preston +1 more
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