Back to Search
Start Over
AbĀ Initio Multiplet-Plus-Cumulant Approach for Correlation Effects in X-Ray Photoelectron Spectroscopy.
- Source :
-
Physical review letters [Phys Rev Lett] 2022 May 27; Vol. 128 (21), pp. 216401. - Publication Year :
- 2022
-
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.
Details
- Language :
- English
- ISSN :
- 1079-7114
- Volume :
- 128
- Issue :
- 21
- Database :
- MEDLINE
- Journal :
- Physical review letters
- Publication Type :
- Academic Journal
- Accession number :
- 35687432
- Full Text :
- https://doi.org/10.1103/PhysRevLett.128.216401