Related papers: Ehrenfest dynamics accelerated with SPEED
Treated traditionally by the Ehrenfest approximation, dynamics of a one-dimensional molecular crystal model with off-diagonal exciton-phonon coupling is investigated in this work using the Dirac-Frenkel time-dependent variational principle…
The Ehrenfest dynamics, representing a quantum-classical mean-field type coupling, is a widely used approximation in quantum molecular dynamics. In this paper, we propose a time-splitting method for an Ehrenfest dynamics, in the form of a…
Linear and nonlinear electronic spectra provide an important tool to probe the absorption and transfer of electronic energy. Here we introduce a pure state Ehrenfest approach to obtain accurate linear and nonlinear spectra that is…
Recently introduced methods which result in shortcuts to adiabaticity, particularly in the context of frictionless cooling, are rederived and discussed in the framework of an approach based on Ehrenfest dynamics. This construction provides…
Simulating electron-ion dynamics using time-dependent density functional theory within an Ehrenfest dynamics scheme can be done in two ways that are in principle exact and identical: propagating time-dependent electronic Kohn-Sham equations…
Mixed-quantum classical (MQC) methods for simulating the dynamics of molecules at metal surfaces have the potential to accurately and efficiently provide mechanistic insight into reactive processes. Here, we introduce simple two-dimensional…
Nonadiabatic transition dynamics lies at the core of many electron/hole transfer, photoactivated, and vacuum field-coupled processes. About a century after Ehrenfest proposed "Phasenraum" and the Ehrenfest theorem, we report a conceptually…
We propose to measure nonadiabaticity of molecular quantum dynamics rigorously with the quantum fidelity between the Born-Oppenheimer and fully nonadiabatic dynamics. It is shown that this measure of nonadiabaticity applies in situations…
We present a Lagrangian-based implementation of Ehrenfest dynamics with nuclear-electronic orbital (NEO) theory and real-time time-dependent density functional theory (RT-TDDFT) for extended periodic systems. In addition to a quantum…
The atomistic resolution recently achieved by ultrafast spectroscopies demands corresponding theoretical advances. Real-time time-dependent density-functional theory (RT-TDDFT) with Ehrenfest dynamics offers an optimal trade-off between…
Mixed-quantum-classical molecular dynamics simulation implies an effective measurement on the electronic states owing to continuously tracking the atomic forces.Based on this insight, we propose a quantum trajectory mean-field approach for…
The approach of shortcuts to adiabaticity enables the effective execution of adiabatic dynamics in quantum information processing with enhanced speed. Owing to the inherent trade-off between dynamical speed and the cost associated with the…
A new "on the fly" method to perform Born-Oppenheimer ab initio molecular dynamics (AIMD) is presented. Inspired by Ehrenfest dynamics in time-dependent density functional theory, the electronic orbitals are evolved by a Schroedinger-like…
An accurate description of nonadiabatic dynamics of molecular species on metallic surfaces poses a serious computational challenge associated with a multitude of closely-spaced electronic states. We propose a mixed quantum-classical scheme…
A multilevel approach to sample the potential energy surface in a path integral formalism is proposed. The purpose is to reduce the required number of ab initio evaluations of energy and forces in ab initio path integral molecular dynamics…
Injection from metallic electrodes serves as a main channel of charge generation in organic semiconducting devices and the quantum effect is normally regarded to be essential. We develop a dynamic approach based upon the surface hopping…
Collisions of atoms and molecules with metal surfaces create electronic excitations in the metal, leading to nonadiabatic energy dissipation, inelastic scattering, and sticking. Mixed quantum-classical molecular dynamics simulation methods,…
Experiments indicate that collective coupling of molecular ensembles to confined optical modes can modify excited-state dynamics and photochemical reactivity. To describe such cavity-induced effects at atomic resolution, semi-classical…
We present a dynamical simulation scheme to model the highly correlated excited state dynamics of linear polyenes. We apply it to investigate the internal conversion processes of carotenoids following their photoexcitation. We use the…
We describe vacuum fluctuations and photon-field correlations in interacting quantum mechanical light-matter systems, by generalizing the application of mixed quantum-classical dynamics techniques. We employ the multi-trajectory…