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
More filters
Journal ArticleDOI
A general method to describe intersystem crossing dynamics in trajectory surface hopping
TL;DR: In this paper, a general trajectory surface hopping methodology, termed SHARC, which is able to include nonadiabatic and spin-orbit couplings in excited state dynamics simulations, is explained in detail.
Journal ArticleDOI
Tensor product methods and entanglement optimization for ab initio quantum chemistry
Szilárd Szalay,Max Pfeffer,Valentin Murg,Gergely Barcza,Frank Verstraete,Reinhold Schneider,Örs Legeza +6 more
TL;DR: In this article, the authors present general techniques that can be used for the treatment of high-dimensional optimization tasks and time-dependent equations, and connect them to concepts already used in many-body quantum physics.
Book
Tensor Networks for Dimensionality Reduction and Large-scale Optimization: Part 1 Low-Rank Tensor Decompositions
TL;DR: In this paper, the authors provide innovativesolutions to low-rank tensor network decompositions and easy to interpretgraphical representations of the mathematical operations ontensor networks, and demonstrate the ability of tensor networks to provide linearly or even super-linearly e.g., logarithmically scalablesolutions, as illustrated in detail in Part 2.
Journal ArticleDOI
Exciton–vibrational coupling in the dynamics and spectroscopy of Frenkel excitons in molecular aggregates
Marco Schröter,Sergei D. Ivanov,Jan Schulze,Sergey Polyutov,Sergey Polyutov,Yun-An Yan,Tõnu Pullerits,Oliver Kühn +7 more
TL;DR: In this article, the authors summarized the state of the art of the theory of exciton-vibrational interaction in molecular aggregates and photosynthetic antenna complexes and put on the discussion of the basic effects of the interaction from the stationary and dynamics points of view.
Journal ArticleDOI
Theory and Simulation of the Ultrafast Double-Bond Isomerization of Biological Chromophores.
TL;DR: An overview of state-of-the-art computational studies on subnanosecond events in rhodopsins, photoactive yellow proteins, phytochromes, and some other photoresponsive proteins where photoinduced double-bond isomerization occurs is presented.
References
More filters
Journal ArticleDOI
Light-Induced Redox Reactions in Nanocrystalline Systems
Anders Hagfeldt,Michael Graetzel +1 more
TL;DR: A review with 156 refs on interfacial electron transfer reactions in colloidal semiconductor solns and thin films and their application for solar light energy conversion and photocatalytic water purifn is presented in this paper.
Journal ArticleDOI
Dynamics of the dissipative two-state system
Anthony J. Leggett,Sudip Chakravarty,Alan T. Dorsey,Matthew P. A. Fisher,Anupam Garg,Wilhelm Zwerger +5 more
TL;DR: In this article, a functional-integral approach to the dynamics of a two-state system coupled to a dissipative environment is presented, and an exact and general prescription for the reduction, under appropriate circumstances, of the problem of a system tunneling between two wells in the presence of dissipative environments to the spin-boson problem is given.
Book
Quantum Dissipative Systems
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
Journal ArticleDOI
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.