Speeding up all-electron real-time TDDFT demonstrated by the exciting package

Abstract

Currently, many ab initio codes are being prepared for exascale computing. A first and important step is to significantly improve the efficiency of existing implementations by devising better algorithms that can accomplish the same tasks with enhanced scalability. This manuscript addresses this challenge for real-time time-dependent density functional theory in the full-potential all-electron code exciting, with a focus on systems with reduced dimensionality. Following the strategy described here, calculations can run orders of magnitude faster than before. We demonstrate this with the molecules H$_2$ and CO, achieving speedups between 98 to over 50,000. We also present an example where conventional calculations would be particularly costly, namely the inorganic/organic heterostructure of pyridine physisorbed on monolayer MoS$_2$.