Real-Time TDDFT Using Noncollinear Functionals

J Chem Theory Comput. 2024 Dec 10;20(23):10477-10490. doi: 10.1021/acs.jctc.4c01218. Epub 2024 Nov 27.

Abstract

Recently, we proposed a method to generalize collinear functionals to noncollinear functionals, called multicollinear approach, which has been applied in density functional theory (DFT) and linear-response time-dependent DFT (TDDFT) for the ground state and excited states calculations, respectively. In this work, we demonstrate the application of this method in real-time TDDFT by simulating electronic absorption spectra, Rabi resonance, and precession of a two-magnetic center system. Thanks to the nonvanishing local exchange-correlation torque provided by multicollinear functionals, research into the torques in the evolution of magnetization vector is carried out, which is useful for the exploration on spin dynamics.