Nonlocal and nonadiabatic Pauli potential for time-dependent orbital-free density functional theory

Abstract

Time-dependent orbital-free density functional theory (TD-OFDFT) is an efficient ab-initio method for calculating the electronic dynamics of large systems. In comparison to standard TD-DFT, it computes only a single electronic state regardless of system size, but it requires an additional time-dependent Pauli potential term. We propose a nonadiabatic and nonlocal Pauli potential whose main ingredients are the time-dependent particle and current densities. Our calculations of the optical spectra of metallic and semiconductor clusters indicate that nonlocal and nonadiabatic TD-OFDFT performs accurately for metallic systems and semiquantitatively for semiconductors. This work opens the door to wide applicability of TD-OFDFT for nonequilibrium electron and electron-nuclear dynamics of materials.

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• Nonlocal Orbital-Free Kinetic Energy Functional from the Jellium-with-Gap Model for Finite Systems
• Density-Functional-Theory Perspective on the Non-Linear Response of Correlated Electrons Across Temperature Regimes