Efficient time-dependent orbital-free density functional theory: Semilocal adiabatic response
Kaili Jiang, Xuecheng Shao, Michele Pavanello
Abstract
Orbital-free density functional theory and its time-dependent extension are efficient ab initio methods for calculating the electronic structure and dynamics of large systems. Through the calculation of the optical spectra of selected clusters, we reach three important conclusions: (1) The quality of the spectra is strongly affected by the quality of the corresponding ground-state electron density; (2) the adiabatic part of the electronic response to external perturbations can be safely evaluated at the semilocal level; and (3) the nonadiabatic, current-dependent part of the time-dependent Pauli potential is key to recover correct spectral envelopes.
Topics & Concepts
Adiabatic processPhysicsPauli exclusion principleDensity functional theoryAb initioTime-dependent density functional theoryQuality (philosophy)Spectral lineAtomic physicsQuantum mechanicsAdvanced Chemical Physics StudiesMolecular Junctions and NanostructuresSpectroscopy and Quantum Chemical Studies