Real-time TDDFT for complex systems and dynamics

Real-time propagation approach to time-dependent density functional theory (RT-TDDFT) is a powerful first-principles method for simulating nonequilibrium electron dynamics. I will start by discussing our method development effort, particularly how massively-parallel computers are used to investigate electron dynamics in large complex systems like DNA solvated in water under ion irradiation. I will then discuss the need for advanced hybrid exchange-correlation approximations in the context of RT-TDDFT and how the unitary transformation of time-dependent orbitals is used to mitigate their prohibitively large cost for condensed matter systems. I will finish the talk by discussing our new effort on using nuclear-electronic orbital (NEO) paradigm for expanding the realm of RT-TDDFT by treating protons quantum-mechanically in heterogeneous systems. Competing kinetics between electronic excitation dynamics and quantum-mechanical proton transfer is discussed as an example of how such new multicomponent DFT formulation can expand the application of RT-TDDFT.