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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Book ChapterDOI
Time‐Dependent Approaches to Calculation of Steady‐State Vibronic Spectra: From Fully Quantum to Classical Approaches
Alessandro Lami,Fabrizio Santoro +1 more
Journal ArticleDOI
Numerical assessment for accuracy and GPU acceleration of TD-DMRG time evolution schemes.
TL;DR: This paper comparatively studies the accuracy of three time evolution schemes in the TD-DMRG, the global propagation and compression method with the Runge-Kutta algorithm, the time dependent variational principle based methods with the matrix unfolding algorithm, and with the projector-splitting algorithm by performing benchmarks on the exciton dynamics of the Fenna-Matthews-Olson complex.
Journal ArticleDOI
Improved on-the-Fly MCTDH Simulations with Many-Body-Potential Tensor Decomposition and Projection Diabatization
TL;DR: The efficiency and accuracy of DD-MCTDH can be dramatically improved further still by using systematic tensor decompositions of the KRR PES, and using a novel scheme for diabatization within the framework of configuration interaction methods which only requires local adiabatic electronic states, rather than non-adiabatic coupling matrix elements.
Book ChapterDOI
Tensor Spaces and Hierarchical Tensor Representations
TL;DR: It is highlighted that the present tensor representations are constituting smooth manifolds, and a perspective how these properties can be used to develop numerical solvers for tensor equations and tensor optimisation problems.
Journal ArticleDOI
Nonadiabatic quantum-classical reaction rates with quantum equilibrium structure
Hyojoon Kim,Raymond Kapral +1 more
TL;DR: Time correlation function expressions for quantum reaction-rate coefficients are computed in a quantum-classical limit and approximate analytical expressions for the spectral density function, which incorporate quantum effects in the many-body environment and reaction coordinate, are derived.
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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