PNNL

Abstract

Real-time electronic structure methods provide an unprecedented view of electron dynamics and ultrafast spectroscopy on the atto and femtosecond timescale, with vast potential to yield new insights into the electronic behavior of molecules and materials. In this Review, we discuss the fundamental theory underlying various real-time elec- tronic structure methods, as well as advantages and disadvantages of each. We give an overview of the numerical techniques that are widely used for real-time propagation of the quantum electron dynamics, with an emphasis on Gaussian basis set methods. We also showcase many of the chemical applications and scientific advances made by using real-time electronic structure calculations and provide an outlook of possible new directions.