Ehrenfest dynamics with localized atomic-orbital basis sets within the projector augmented-wave method

Abstract

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 the Ehrenfest molecular dynamics (ED) method with the approximate approach of Tomfohr and Sankey within the projector augmented-wave code GPAW. We apply this method to small molecules as well as larger periodic systems, and elucidate its limits, advantages, and disadvantages in comparison to the existing implementation of Ehrenfest dynamics with a real-space grid representation. For modest atomic velocities, LCAO-ED shows satisfactory accuracy at a much reduced computational cost. This method will be particularly useful for modeling ion irradiation processes that require large amounts of vacuum in the simulation cell.

References in corpus (12)

• CP2K: An Electronic Structure and Molecular Dynamics Software Package -- Quickstep: Efficient and Accurate Electronic Structure Calculations
• SIESTA: recent developments and applications
• Localized atomic basis set in the projector augmented wave method
• GPAW: An open Python package for electronic-structure calculations
• Localized surface plasmon resonance in silver nanoparticles: Atomistic first-principles time-dependent density-functional theory calculations
• Time-Dependent Density Functional Theory with Ultrasoft Pseudopotential: Real-Time Electron Propagation across Molecular Junction
• Electronic stopping power in a narrow band gap semiconductor from first principles
• Nonadiabatic Ehrenfest molecular dynamics within the projector augmented-wave method
• Anomalous stopping and charge transfer in proton-irradiated graphene
• Anisotropy of electronic stopping power in graphite
• Propagation of maximally localized Wannier functions in real-time TDDFT
• Quantum mechanics in an evolving Hilbert space

Cited by in corpus (1)

• Diffraction of atomic matter waves through a 2D crystal