Ab Initio Multiplet-Plus-Cumulant Approach for Correlation Effects in X-Ray Photoelectron Spectroscopy.
Phys Rev Lett
; 128(21): 216401, 2022 May 27.
Article
em En
| MEDLINE
| ID: mdl-35687432
ABSTRACT
The treatment of electronic correlations in open-shell systems is among the most challenging problems of condensed matter theory. Current approximations are only partly successful. Ligand-field multiplet theory has been widely successful in describing intra-atomic correlation effects in x-ray spectra, but typically ignores itinerant states. The cumulant expansion for the one-electron Green's function has been successful in describing shake-up effects but ignores atomic multiplets. More complete methods, such as dynamic mean-field theory can be computationally demanding. Here, we show that separating the dynamic Coulomb interactions into local and longer-range parts with ab initio parameters yields a combined multiplet-plus-cumulant approach that accounts for both local atomic multiplets and satellite excitations. The approach is illustrated in transition metal oxides and explains the multiplet peaks, charge-transfer satellites, and distributed background features observed in XPS experiment.
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MEDLINE
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En
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Phys Rev Lett
Ano de publicação:
2022
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Article