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
Colloquium : Multiconfigurational time-dependent Hartree approaches for indistinguishable particles
TL;DR: In this article, a theory and associated practical numerical approaches to treat the time-dependent Schrodinger equation for identical interacting particles from first principles and their use in atomic and molecular systems are discussed.
Journal ArticleDOI
Challenges facing an understanding of the nature of low-energy excited states in photosynthesis.
Jeffrey R. Reimers,Jeffrey R. Reimers,Malgorzata Biczysko,Douglas Bruce,David F. Coker,Terry J. Frankcombe,Hideki Hashimoto,Jürgen Hauer,Ryszard Jankowiak,Tobias Kramer,Juha Linnanto,Fikret Mamedov,Frank Müh,Margus Rätsep,Thomas Renger,Stenbjörn Styring,Jian Wan,Zhuan Wang,Zheng-Yu Wang-Otomo,Yuxiang Weng,Chunhong Yang,Jian-Ping Zhang,Arvi Freiberg,Elmars Krausz +23 more
TL;DR: A concerted experimental and theoretical research strategy is suggested and outlined, this being aimed at providing a fully comprehensive understanding of low-energy states in photochemical systems.
Journal ArticleDOI
Numerically exact, time-dependent treatment of vibrationally coupled electron transport in single-molecule junctions.
TL;DR: The multilayer multiconfiguration time-dependent Hartree (ML-MCTDH) theory within second quantization representation of the Fock space, a novel numerically exact methodology to treat many-body quantum dynamics for systems containing identical particles, is applied to study the effect of vibrational motion on electron transport in a generic model for single-molecule junctions.
Journal ArticleDOI
Iterative diagonalization in the state-averaged multi-configurational time-dependent Hartree approach: excited state tunneling splittings in malonaldehyde.
Thorsten Hammer,Uwe Manthe +1 more
TL;DR: An iterative block Lanczos-type diagonalization scheme utilizing the state-averaged multi-configurational time-dependent Hartree (MCTDH) approach is introduced and results for the tunneling splittings of several excited vibrational states can be obtained.
Journal ArticleDOI
Quantum-mechanical evaluation of the Boltzmann operator in correlation functions for large molecular systems: a multilayer multiconfiguration time-dependent Hartree approach.
Haobin Wang,Michael Thoss +1 more
TL;DR: It is shown that the Boltzmann operator in time correlation functions for complex molecular systems can be evaluated in a numerically exact way employing the multilayer formulation of the multiconfiguration time-dependent Hartree theory in combination with Monte Carlo importance sampling techniques.
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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