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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Nanosized Carbon Particles From Natural Gas Soot
TL;DR: In this paper, carbon nanoparticles were prepared by refluxing the combustion soot of natural gas in nitric acid and the resulting particles exhibited an average diameter of 4.8 ± 0.6 nm, and the crystalline lattices were consistent with graphitic carbons.
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A literature survey of low-rank tensor approximation techniques
TL;DR: This survey attempts to give a literature overview of current developments in low-rank tensor approximation, with an emphasis on function-related tensors.
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Hierarchical Singular Value Decomposition of Tensors
TL;DR: This hierarchical SVD has properties like the matrix SVD (and collapses to the SVD in $d=2$), and it is proved that one can find low rank (almost) best approximations in a hierarchical format ($\mathcal{H}$-Tucker) which requires only $\ mathcal{O}((d-1)k^3+dnk)$ parameters.
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Perspective: Nonadiabatic dynamics theory.
TL;DR: This Perspective examines the most significant theoretical and computational obstacles to achieving nonadiabatic dynamics realism, and suggests some possible strategies that may prove fruitful.
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Spin-Vibronic Mechanism for Intersystem Crossing
TL;DR: The theory and fundamental principles of the spin-vibronic mechanism for ISC are presented, followed by empirical rules to estimate the rate of ISC within this regime.
References
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Journal ArticleDOI
A theory for adiabatic electron transfer processes across the semiconductor/electrolyte interface
Yuri G. Boroda,Gregory A. Voth +1 more
TL;DR: A theory for adiabatic electron transfer between a semiconductor electrode and an electron acceptor species in a polar electrolyte is developed by extending the Anderson-Newns model as adapted for metal/electrolyte interfaces as mentioned in this paper.
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Theory of vibrational relaxation processes in resonant collisions of low-energy electrons with large molecules
Michael Thoss,Wolfgang Domcke +1 more
TL;DR: In this article, the effect of intramolecular vibrational relaxation in resonant collisions of low-energy electrons with large molecules is investigated, and the theory is formulated within the framework of the projection operator formalism.
Journal ArticleDOI
Quantum dynamical simulation of ultrafast photoinduced electron transfer processes in a mixed-valence compound
Michael Thoss,Haobin Wang +1 more
TL;DR: In this paper, a self-consistent hybrid method was applied to a model that is based on the analysis of optical line shapes by Barbara and coworkers to investigate the dynamics of the back electron transfer after photoexcitation.
Journal ArticleDOI
Recursive evaluation of the real-time path integral for dissipative systems. The spin-boson model
TL;DR: In this paper, a real-time path-integral approach is proposed for the tunneling dynamics of an electronic two-state system coupled to a bath of harmonic oscillators at zero temperature.
Journal ArticleDOI
Discretization of the electron continuum in the non-local theory of inelastic electron - molecule collisions
TL;DR: In this article, the basic integral equation of the non-local theory of inelastic resonant electron - molecule collisions is recast in the form of a system of differential equations for a set of the electron resonance pseudostates.