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
Novel perspectives in quantum dynamics
TL;DR: In this article, the authors focus on novel methods which can provide predictions for medium-sized and large systems and on the difficulties encountered when facing the huge dimension of the primitive basis within a quantum mechanical framework.
Journal ArticleDOI
Nanosized carbon dots from organic matter and biomass
Yuanyuan Li,Tong Chen,Yulong Ma +2 more
TL;DR: In this paper, carbon nanoparticles (C-dots) were prepared by refluxing the combustion soots of candles and corn stalks in nitric acid, and two kinds of Cdots all exhibited unique photoluminescent properties.
Journal ArticleDOI
WavePacket: A Matlab package for numerical quantum dynamics. III. Quantum-classical simulations and surface hopping trajectories.
TL;DR: The present work describes the MATLAB version of WavePacket 6.1.0, which is essentially an object‐oriented rewrite of previous versions, allowing to perform fully classical, quantum‐classical and quantum‐mechanical simulations on an equal footing, that is, for the same physical system described by the same WavePackets input.
Journal ArticleDOI
Rigorous close-coupling quantum dynamics calculation of thermal rate constants for the water formation reaction of H2 + OH on a high-level PES.
TL;DR: It is found that the J-shifting approximation works well for the title reaction given that a high-level PES is used for the dynamics calculation and the importance of treating the spin-orbit coupling in the reactant partition function is discussed.
Quantized-TT-Cayley transform to compute dynamics and spectrum of high-dimensional Hamiltonians
TL;DR: A class of tensor methods for the efficient numerical computation of dynamics and spectrum of high-dimensional Hamiltonians is proposed and analysed and it is shown that the spectrum of Hamiltonian can also be represented by the poles of the t-Laplace transform of a solution.
References
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Light-Induced Redox Reactions in Nanocrystalline Systems
Anders Hagfeldt,Michael Graetzel +1 more
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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
TL;DR: In this article, an extension of the classical trajectory approach is proposed that may be useful in treating many types of nonadiabatic molecular collisions, where nuclei are assumed to move classically on a single potential energy surface until an avoided surface crossing or other region of large NDE coupling is reached.