The time-dependent generalized active space configuration interaction approach to correlated ionization dynamics of diatomic molecules

Progress in Non-equilibrium Green's Functions

Bauch, S.^1 ; Larsson, H.R.^2 ; Hinz, C.^1 ; Bonitz, M.^1

Institute for Theoretical Physics and Astrophysics, Christian-Albrechts-Universität Kiel, Kiel

24098, Germany^1

Institute for Physical Chemistry, Christian-Albrechts-Universität Kiel, Kiel

24098, Germany^2

关键词: Configuration interactions;    Electron correlation effect;    Electron-electron correlation;    Linearly polarized laser field;    Many body wave functions;    Photoionization dynamics;    Reference descriptions;    Strong field ionization;   

Others  :  https://iopscience.iop.org/article/10.1088/1742-6596/696/1/012008/pdf
DOI  :  10.1088/1742-6596/696/1/012008

来源: IOP

【 摘 要 】

In this contribution, we review the time-dependent generalized-active-space configuration interaction (TD-GAS-CI) approach to the photoionization dynamics of atoms and molecules including electron correlation effects. It is based on the configuration interaction (CI) expansion of the many-body wave function and the restriction of the determinantal space to a reduced subspace. For its numerically efficient application to photoionization, a partially-rotated basis set is used which adopts features of a localized basis with a good reference description and a grid representation for escaping wave packets. After reviewing earlier applications of the theory, we address the strong-field ionization of a one-dimensional model of the four-electron LiH molecule using TD-GAS-CI and demonstrate the importance of electron-electron correlations in the ionization yield for different orientations of the molecule w.r.t the peak of the linearly polarized laser field. A pronounced orientation-dependent variation of the yield with the pulse duration and the level of considered electron-electron correlations is observed.