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Quasi-Diabatic Representation for Nonadiabatic Dynamics Propagation
journal contribution
posted on 2018-02-28, 00:00 authored by Arkajit Mandal, Sharma SRKC Yamijala, Pengfei HuoWe develop a nonadiabatic dynamics
propagation scheme that allows
interfacing diabatic quantum dynamics methods with commonly used adiabatic
electronic structure calculations. This scheme uses adiabatic states
as the quasi-diabatic (QD) states during a short-time quantum dynamics
propagation. At every dynamical propagation step, these QD states
are updated based on a new set of adiabatic basis. Using the partial
linearized density matrix (PLDM) path-integral method as one specific
example for diabatic dynamics approaches, we demonstrate the accuracy
of the QD scheme with a wide range of model nonadiabatic systems as
well as the on-the-fly propagations with density functional tight-binding
(DFTB) calculations. This study opens the possibility to combine accurate
diabatic quantum dynamics methods with adiabatic electronic structure
calculations for nonadiabatic dynamics propagations.
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nonadiabatic dynamics propagationsnonadiabatic dynamics propagation schemeDFTBPLDMinterfacing diabatic quantum dynamics methodslinearized density matrixNonadiabatic Dynamics Propagationdiabatic dynamics approachesmodel nonadiabatic systemsdiabatic quantum dynamics methodsquantum dynamics propagationQDstructure calculations