Real time cumulant approach for charge-transfer satellites in x-ray photoemission spectra
X-ray photoemission spectra generally exhibit satellite features in addition to quasi-particle peaks due to many-body excitations which have been of considerable theoretical and experimental interest. However, the satellites attributed to charge-transfer (CT) excitations in correlated materials have proved difficult to calculate from first principles. Here we report a real-time, real-space approach for such calculations based on a cumulant representation of the core-hole Green’s function and time-dependent density functional theory. This approach also yields an interpretation of CT satellites in terms of a complex oscillatory, transient response to a suddenly created core hole. Illustrative results for TiO2 and NiO are in good agreement with experiment.
- Research Organization:
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
- Sponsoring Organization:
- USDOE
- DOE Contract Number:
- AC05-76RL01830
- OSTI ID:
- 1208739
- Report Number(s):
- PNNL-SA-104564; 48341; KC0203020
- Journal Information:
- Physical Review. B, Condensed Matter, 91(12):Article No. 121112(R), Journal Name: Physical Review. B, Condensed Matter, 91(12):Article No. 121112(R)
- Country of Publication:
- United States
- Language:
- English
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