The importance of nonlocality and nonadiabaticity in the Pauli potential for time-dependent orbital-free density functional theory
Year: 2021
Type: preprint
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 only requires the computation of a single electronic state regardless of system size, therefore ridding the computation of many electronic states. In addition to the usual effective, time-dependent Kohn-Sham Hamiltonian, the time-dependent Pauli potential is needed. Based on our recently proposed nonadiabatic Pauli kernel, we present a nonadiabatic correction to the 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 TD-OFDFT recovers the overall spectral envelope for these systems provided that space and time nonlocality are both included in the model.
Source: arXiv (Cornell University)
Authors: Kaili Jiang, Michele Pavanello
Language: English
Subfield: Atomic and Molecular Physics, and Optics
Field: Physics and Astronomy
Domain: Physical Sciences
Open Access status: green
OpenAlex ID: W3196280993