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Quasi-Diabatic Representation for Nonadiabatic Dynamics Propagation
journal contributionposted on 2018-02-28, 00:00 authored by Arkajit Mandal, Sharma SRKC Yamijala, Pengfei Huo
We 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.
nonadiabatic dynamics propagationsnonadiabatic dynamics propagation schemeDFTBPLDMinterfacing diabatic quantum dynamics methodslinearized density matrixNonadiabatic Dynamics Propagationdiabatic dynamics approachesmodel nonadiabatic systemsdiabatic quantum dynamics methodsquantum dynamics propagationQDstructure calculations