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arXiv · 1803.01512

Quasiparticle energy spectra of isolated atoms from coupled-cluster singles and doubles (CCSD): Comparison with exact CI calculations

Hirofumi Nishi·Taichi Kosugi·Yoritaka Furukawa·Yu-ichiro Matsushita
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Abstract

In this study, we have calculated single-electron energy spectra via the Green's function based on the coupled-cluster singles and doubles (GFCCSD) method for isolated atoms from H to Ne. In order to check the accuracy of the GFCCSD method, we compared the results with the exact ones calculated from the full-configuration interaction (FCI). Consequently, we have found that the GFCCSD method reproduces not only the correct quasiparticle peaks but also satellite ones by comparing the exact spectra with the 6-31G basis set. It is also found that open-shell atoms such as C atom exhibit Mott gaps at the Fermi level, which the exact density-functional theory (DFT) fails to describe. The GFCCSD successfully reproduces the Mott HOMO-LUMO (highest-occupied molecular orbital and lowest-unoccupied molecular orbital) gaps even quantitatively. We also discussed the origin of satellite peaks as shake-up effects by checking the components of wave function of the satellite peaks. The GFCCSD is a novel cutting edge to investigate the electronic states in detail.

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Hirofumi Nishi, Taichi Kosugi, Yoritaka Furukawa, Yu-ichiro Matsushita. 2018-03-05. Quasiparticle energy spectra of isolated atoms from coupled-cluster singles and doubles (CCSD): Comparison with exact CI calculations. https://doi.org/10.1063/1.5029536

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