Ultrafast spectroscopy is one of the main driving forces to develop realtime (RT) electronic structure methods. Realtime mean field theories such as RT-TDDFT and RT-TDHF dominate applications because of the speed required to access picosecond timescales. Yet TDHF and TDDFT are not accurate enough to properly model resonant driving, which is only one ingredient in ultrafast spectroscopy. In this talk I discuss a simple density-matrix equation of motion implemented as an approximation to RT-TDDFT, which excites properly on resonance. Based on this foundation I compare the non-equilibrium steady states of the correct DFT and a Markovian bath model, with essentially exact results coming from HEOM showing that TDDFT can be used to study driven ultrafast dynamics. I then discuss self-consistency in correlated corrections to TDDFT which have low cost and can be applied to large systems.

Patches for realtime TDDFT: Correlation and a time-dependent Tamm-Dancoff approximation

253rd National Meeting (2017)

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