Reformulation of Time-Dependent Density Functional Theory for Non-Perturbative Dynamics: The Rabi Oscillation Problem Resolved

2024/04/22 by Davood B. Dar, Dar, Davood B., Anna A. Baranova +3 · 5 citations
Mathematics · Physics and Astronomy · #Advanced Thermodynamics and Statistical Mechanics #Atomic Physics (physics.atom-ph) #Chemical Physics (physics.chem-ph) #Computational Physics (physics.comp-ph) #FOS: Physical sciences #Gas Dynamics and Kinetic Theory #Quantum Electrodynamics and Casimir Effect

paper · pdf · doi:10.48550/arxiv.2404.14505

openalex publication_date 2024/04/22 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28

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.

Cited by

• Low-energy proton impact dynamics on hydrocarbons: Dependence on kinetic energy and incident site
• A Snapshot of Time-Dependent Density-Functional Theory
• Electron charge dynamics and charge separation: A response theory approach
• Plasmon-assisted photoelectron emission in a model cluster using time-dependent density functional theory and the time-dependent surface-flux method
• Ensemble Time-Dependent Density Functional Theory

Related

• Prevalence of the adiabatic exchange-correlation potential approximation in time-dependent density functional theory
• Linear response and resonances in adiabatic time-dependent density functional theory
• Harnessing dressed time-dependent density functional theory for the non-perturbative regime: Electron dynamics with double excitations
• A Snapshot of Time-Dependent Density-Functional Theory
• Time-dependent density functional theory: Past, present, and future