We develop the quasi-diabatic (QD) propgation scheme to directly interface diabatic quantum dynamics methods with adiabatic outputs of any electronic structure approach. The QD scheme constructs a compact local diabatic representation using the adiabatic states at the present nuclear configuration and then updates them at every dynamical propagation step. The QD scheme extends the scope and applicability of diabatic quantum dynamics approaches, enabling us to combine them with any adiabatic electronic structure method for direct quantum dynamics propagation, alleviating non-trivial efforts of diabatization or reformulation of diabatic quantum dynamics methods. We use this method to simulate new chemical reactivities induced by cavity quantum electrodynamics, where light-matter eigenstates, the polaritonic states are used to propagate dynamics with the QD scheme. Using this approach we also investigate the mechanistic details of a proton coupled electron transfer reaction.

On-the-fly quantum dynamics simulation with quasi-diabatic propagation scheme

ACS Fall 2021

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