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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Computational and data driven molecular material design assisted by low scaling quantum mechanics calculations and machine learning
TL;DR: In this paper, a review of low-scale ground-state and excited-state QM approaches and their applications to long oligomers, self-assembled supramolecular complexes, stimuli-responsive materials, mechanically interlocked molecules, and excited state processes in molecular aggregates are presented.
Journal ArticleDOI
The role of vibronic coupling in the electronic spectroscopy of maleimide: a multi-mode and multi-state quantum dynamics study.
TL;DR: The first two excitation bands below 7 eV in the electronic absorption spectrum of maleimide are investigated using a model Hamiltonian including four low-lying singlet excited states within the manifold of 24 vibrational modes.
Journal ArticleDOI
Extended vibrational coupled cluster: Stationary states and dynamics.
TL;DR: The results highlight the importance of exponential parameterizations and separability in general, as seen, in particular, for the TDEVCC bra parameterization, which is in contrast to the partially linear one of TDVCC.
Journal ArticleDOI
Real-time non-adiabatic dynamics in the one-dimensional Holstein model: Trajectory-based vs exact methods.
M. Ten Brink,Stefan Gräber,Miroslav Hopjan,David Jansen,Jan Stolpp,Fabian Heidrich-Meisner,Peter E. Blöchl +6 more
TL;DR: In this paper , a set of quantum-chemistry methods, including multitrajectory Ehrenfest, fewest-switches surface-hopping, and multiconfigurational-Ehrenfest dynamics, are compared against exact quantum-many-body techniques by studying real-time dynamics in the Holstein model.
Journal ArticleDOI
Nonequilibrium charge transport through Falicov-Kimball structures connected to metallic leads
Martin Žonda,Michael Thoss +1 more
TL;DR: In this paper, a sign-problem-free Monte Carlo approach and nonequilibrium Green's-function techniques were employed to study the transport characteristics of a two-dimensional spinless Falicov-Kimball system coupled to two noninteracting leads.
References
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The multiconfiguration time-dependent Hartree (MCTDH) method: a highly efficient algorithm for propagating wavepackets
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Trajectory Surface Hopping Approach to Nonadiabatic Molecular Collisions: The Reaction of H+ with D2
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