In this study, we developed an efficient time-dependent complete active space configuration interaction (TD-CASCI) method based on a direct s-vector formation algorithm which is accelerated via graphics processing unit (GPU). We implemented a symplectic split operator to propagate the wavefunction, and the implementation has been validated with d-function pulse and continuous wave to generate accurate molecular absorption spectra (compared to normal CASCI) and Rabi oscillations. In addition, we demonstrated the ability of our method to describe electron dynamics of a large multireference system under intense laser pulses. The simulations of decacene using the 6-31G(d) basis set and a 12 electron/12 orbital active space took 20.1 hours to propagate for 100 femtoseconds with a 1 attosecond time step on a single NVIDIA K40 GPU.

Simulating electron dynamics of complex molecules with time-dependent complete active space configuration interaction

2019 Spring National Meeting

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