Since first introduced to chemical and condensed matter communities through electronic structure theory in 1970s, Green's function based formalisms have been widely exploited in the past few decades to describe molecular electronic structure, compute beyond-ground-state electronic properties, and help interpret the spectra of molecular systems in many emerging physical and chemical areas including photovoltaics, semiconductor, magnetoresistance, and novel superconductivity to name just a few. In this talk, I will present a new working equation for computing spectral functions in the Green's function coupled-cluster (GFCC) framework, and its applications to real molecular systems. The presented method is able to compute the spectral function for a given molecular system in any energy region. Several typical examples have been given to demonstrate its capability of computing spectral functions not only in the valence band, but also in the core-level energy region. Satellite peaks have been observed in the inner valence band and core-level energy region where many-body effect becomes significant and quasiparticle picture of ionization often breaks down. The accuracy test has been carried out by extensively comparing our GFCC results with experimental results as well as the theoretical results from other Green's function based formalisms and some post Hartree-Fock formalisms including equation-of-motion coupled-cluster (EOM-CC) theory and some variants of configuration interaction theory.

Green's function coupled-cluster: Simulating spectral function for real molecular systems

256th National Meeting (2018)

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.