Self-adaptive real-time time-dependent density functional theory for x-ray absorptions

Abstract

Real-time time-dependent density functional theory (RT-TDDFT) can, in principle, access the whole absorption spectrum of a many-electron system exposed to a narrow pulse. However, this requires an accurate and efficient propagator for the numerical integration of the time-dependent Kohn–Sham equation. While a low-order time propagator is already sufficient for the low-lying valence absorption spectra, it is no longer the case for the x-ray absorption spectroscopy (XAS) of systems composed even only of light elements, for which the use of a high-order propagator is indispensable. It is then crucial to choose a largest possible time step and a shortest possible simulation time so as to minimize the computational cost. To this end, we propose here a robust AutoPST approach to determine automatically (Auto) the propagator (P), step (S), and time (T) for relativistic RT-TDDFT simulations of XAS.