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Nonadiabatic Ab Initio Molecular Dynamics with the Floating Occupation Molecular Orbital-Complete Active Space Configuration Interaction Method
We show that the floating occupation
molecular orbital complete
active space configuration interaction (FOMO-CASCI) method is a promising
alternative to the widely used complete active space self-consistent
field (CASSCF) method in direct nonadiabatic dynamics simulations.
We have simulated photodynamics of three archetypal molecules in photodynamics:
ethylene, methaniminium cation, and malonaldehyde. We compared the
time evolution of electronic populations and reaction mechanisms as
revealed by the FOMO-CASCI and CASSCF approaches. Generally, the two
approaches provide similar results. Some dynamical differences are
observed, but these can be traced back to energetically minor differences
in the potential energy surfaces. We suggest that the FOMO-CASCI method
represents, due to its efficiency and stability, a promising approach
for direct ab initio dynamics in the excited state