Time-Dependent Second-Order Green's Function Theory for Neutral Excitations

Wenjie Dou*, Joonho Lee*, Jian Zhu*, Leopoldo Mejía*, David R. Reichman*, Roi Baer*, Eran Rabani*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

2 Scopus citations

Abstract

We develop a time-dependent second-order Green's function theory (GF2) for calculating neutral excited states in molecules. The equation of motion for the lesser Green's function (GF) is derived within the adiabatic approximation to the Kadanoff-Baym (KB) equation, using the second-order Born approximation for the self-energy. In the linear response regime, we recast the time-dependent KB equation into a Bethe-Salpeter-like equation (GF2-BSE), with a kernel approximated by the second-order Coulomb self-energy. We then apply our GF2-BSE to a set of molecules and atoms and find that GF2-BSE is superior to configuration interaction with singles (CIS) and/or time-dependent Hartree-Fock (TDHF), particularly for charge-transfer excitations, and is comparable to CIS with perturbative doubles (CIS(D)) in most cases.

Original languageAmerican English
Pages (from-to)5221-5232
Number of pages12
JournalJournal of Chemical Theory and Computation
Volume18
Issue number9
DOIs
StatePublished - 13 Sep 2022

Bibliographical note

Publisher Copyright:
© 2022 American Chemical Society.

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