Real-time, local basis-set implementation of time-dependent density functional theory for excited state dynamics simulations

Abstract

We present a method suitable for large-scale accurate simulations of excited state dynamics within the framework of time-dependent density functional theory (DFT). This is achieved by employing a local atomic basis-set representation and real-time propagation of excited state wave functions. We implement the method within SIESTA, a standard ground-state DFT package with local atomic basis, and demonstrate its potential for realistic and accurate excited state dynamics simulations using small and medium-sized molecules as examples (H-2, CO, O-3, and indolequinone). The method can be readily applied to problems involving nanostructures and large biomolecules.