Nonadiabatic Ehrenfest molecular dynamics within the projector augmented-wave method

Abstract

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 depends on the positions of the nuclei, for example, in atomic orbital basis sets, and in the projector augmented-wave (PAW) method, where the augmentation functions depend on the nuclear positions. We have derived, implemented, and analyzed the energy conserving equations and their most common approximations for a 1D test system where we can achieve numerical results converged to a high accuracy. Based on the observations in 1D, we implement and analyze the Ehrenfest molecular dynamics in 3D using the PAW method and the time-dependent density functional formalism. We demonstrate the applicability of our method by carrying out calculations for small and medium sized molecules in both the adiabatic and the nonadiabatic regime.

12 pages, 10 figures

References in corpus (5)

• A real-space grid implementation of the Projector Augmented Wave method
• A modified Ehrenfest formalism for efficient large-scale ab initio molecular dynamics
• Time-Dependent Density Functional Theory with Ultrasoft Pseudopotential: Real-Time Electron Propagation across Molecular Junction
• Nonadiabatic Ehrenfest molecular dynamics within the projector augmented-wave method
• Ab initio simulations of excited carrier dynamics in carbon nanotubes

Cited by in corpus (15)

• GPAW: An open Python package for electronic-structure calculations
• X-Ray Thomson scattering without the Chihara decomposition
• Nonadiabatic Ehrenfest molecular dynamics within the projector augmented-wave method
• Condensed Matter Systems Exposed to Radiation: Multiscale Theory, Simulations, and Experiment
• Subsystem real-time Time Dependent Density Functional Theory
• All-electron full-potential implementation of real-time TDDFT in exciting
• Improving dynamic collision frequencies: impacts on dynamic structure factors and stopping powers in warm dense matter
• Coupled nuclear and electron dynamics in the vicinity of a conical intersection
• Influence of electronic entropy on Hellmann-Feynman forces in ab initio molecular dynamics with large temperature changes
• Ehrenfest dynamics with localized atomic-orbital basis sets within the projector augmented-wave method
• Ehrenfest dynamics implemented in the all-electron package exciting
• Generation of ultrashort ion pulses from ultrafast electron-stimulated desorption
• Real-Time Time-Dependent Density Functional Theory within FHI-aims
• Photo-induced electronic excitations drive polymerization of carbon monoxide: A first-principles study
• A Unified Heterogeneous Implementation of Numerical Atomic Orbitals-Based Real-Time TDDFT within the ABACUS Package