Related papers: Ehrenfest dynamics implemented in the all-electron…
Real-time time-dependent density functional theory, in conjunction with the Ehrenfest molecular dynamics scheme, is becoming a popular methodology to investigate ultrafast phenomena on the nanoscale. Thanks to recent developments, it is…
Mixed quantum-classical mechanics descriptions are critical to modeling coupled electron-nuclear dynamics, i.e. non-adiabatic molecular dynamics, relevant to photochemical and photophysical processes. We argue that, for polyatomic…
Density functional theory with linear combination of atomic orbitals (LCAO) basis sets is useful for studying large atomic systems, especially when it comes to computationally highly demanding time-dependent dynamics. We have implemented…
We have derived equations for nonadiabatic Ehrenfest molecular dynamics which conserve the total energy in the case of time-dependent discretization for electrons. A discretization is time-dependent in all cases where it or part of it…
Ehrenfest dynamics is a useful approximation for ab initio mixed quantum-classical molecular dynamics that can treat electronically nonadiabatic effects. Although a severe approximation to the exact solution of the molecular time-dependent…
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…
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…
Mixed quantum-classical methods, such as surface hopping and Ehrenfest dynamics, have proven useful for describing molecular processes involving multiple electronic states. These methods require propagating many independent trajectories,…
The increasing need to simulate the dynamics of photoexcited molecular and nanosystems in the sub-picosecond regime demands new efficient tools able to describe the quantum nature of matter at a low computational cost. By combining the…
Processes involving ultrafast laser driven electron-phonon dynamics play a fundamental role in the response of quantum systems in a growing number of situations of interest, as evidenced by phenomena such as strongly driven phase…
A simple formula is obtained for coupling electrons in a complex system to the electromagnetic field. It includes the effect of intra-atomic excitations and nuclear motion, and can be applied in. e.g., first-principles-based simulations of…
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…
The exact nuclear time-dependent potential energy surface arises from the exact decomposition of electronic and nuclear motion, recently presented in [A. Abedi, N. T. Maitra, and E. K. U. Gross, Phys. Rev. Lett. 105, 123002 (2010)]. Such…
The dynamics of an electronic system interacting with an electromagnetic field is investigated within mixed quantum-classical theory. Beyond the classical path approximation (where we ignore all feedback from the electronic system on the…
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…
We use a 1-dimensional tight binding model with an impurity site characterized by electron-vibration coupling, to describe electron transfer and localization at zero temperature, aiming to examine the process of polaron formation in this…
One key challenge in the study of nonadiabatic dynamics in open quantum systems is to balance computational efficiency and accuracy. Although Ehrenfest dynamics (ED) is computationally efficient and well-suited for large complex systems, ED…
We discuss the evolution of purity in mixed quantum/classical approaches to electronic nonadiabatic dynamics in the context of the Ehrenfest model. As it is impossible to exactly determine initial conditions for a realistic system, we…
We consider an Ehrenfest approximation for a particle in a double-well potential in the presence of an external environment schematized as a finite resource heat bath. This allows us to explore how the limitations in the applicability of…
The software package DIALECT is introduced, which provides the capability of calculating excited-state properties and nonadiabatic dynamics of large molecular systems and can be applied to simulate energy and charge-transfer processes in…