We develop a non-adiabatic quantum dynamics propagation scheme that allows interfacing diabatic quantum dynamics approaches with routine adiabatic electronic structure calculations, resolving the challenge of incompatibility between the two methods. This scheme is based on a quasi-diabatic (QD) representation that uses adiabatic states as the quasi-diabatic states during a short-time quantum dynamics propagation. These quasi-diabatic states are updated based on the new set of adiabatic basis at every dynamical propagation step. The QD scheme also provide a numerically stable integration for quantum propagations because it avoids the explicit calculation of the derivative coupling vectors. Using Partial Linearized Density Matrix (PLDM) path-integral method as a specific example for the diabatic dynamics approach, we demonstrate the<br/>accuracy of the QD scheme with model non-adiabatic systems as well as the on-the-fly propagations with Density Functional Tight-Binding (DFTB) calculations. This study opens up the possibility to combine accurate diabatic quantum dynamics methods with routine adiabatic electronic structure calculations for quantum dynamics propagations

Quasi diabatic representation for nonadiabatic quantum dynamics propagation

2019 Spring National Meeting

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