Reformulation of Time-Dependent Density Functional Theory for Non-Perturbative Dynamics: The Rabi Oscillation Problem Resolved
Chemical Physics
2024-06-21 v2 Atomic Physics
Computational Physics
Abstract
Rabi oscillations have long been thought to be out of reach in simulations using time-dependent density functional theory (TDDFT), a prominent symptom of the failure of the adiabatic approximation for non-perturbative dynamics. We present a reformulation of TDDFT which requires response quantities only, thus enabling an adiabatic approximation to predict such dynamics accurately because the functional is evaluated on a density close to the ground-state, instead of on the fully non-perturbative density. Our reformulation applies to it any real-time dynamics, redeeming TDDFT far from equilibrium. Examples of a resonantly-driven local excitation in a model He atom, and charge-transfer in the LiCN molecule are given.
Keywords
Cite
@article{arxiv.2404.14505,
title = {Reformulation of Time-Dependent Density Functional Theory for Non-Perturbative Dynamics: The Rabi Oscillation Problem Resolved},
author = {Davood B. Dar and Anna Baranova and Neepa T. Maitra},
journal= {arXiv preprint arXiv:2404.14505},
year = {2024}
}