Hybridization effect on the x-ray absorption spectra for actinide materials: Application to PuB4
Abstract
Studying the local moment and -electron occupations sheds insight into the electronic behavior in actinide materials. X-ray absorption spectroscopy (XAS) has been a powerful tool to reveal the valence electronic structure when assisted with theoretical calculations. However, the analysis currently taken in the community on the branching ratio of the XAS spectra generally does not account for the hybridization effects between local orbitals and conduction states. In this paper, we discuss an approach which employs the density functional theory plus Gutzwiller rotationally invariant slave boson method to obtain a local Hamiltonian for the single-impurity Anderson model, and calculates the XAS spectra by the exact diagonalization (ED) method. A customized numerical routine was implemented for the ED XAS part of the calculation. By applying this technique to the recently discovered -electron topological Kondo insulator , we determined the signature of -electronic correlation effects in the theoretical x-ray spectra. Furthermore, we found that the Pu hybridization effect provides an extra channel to mix the and orbitals in the valence. As a consequence, the resulting electron occupation number and spin-orbit coupling strength deviate from the intermediate-coupling regime.
- Authors:
-
- Univ. of California, Davis, CA (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Univ. of California, Davis, CA (United States)
- Rutgers Univ., Piscataway, NJ (United States)
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Inst. for Materials Science
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies (CINT)
- Publication Date:
- Research Org.:
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1726189
- Report Number(s):
- LA-UR-20-21956
Journal ID: ISSN 2469-9950
- Grant/Contract Number:
- 89233218CNA000001; FG02-99ER45761; 1411336; SC0014671
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review B
- Additional Journal Information:
- Journal Volume: 102; Journal Issue: 8; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Electronic structure; strongly correlated systems; Anderson impurity model; first-principles calculations; Gutzwiller approximation; numerical techniques; x-ray absorption spectroscopy
Citation Formats
Chiu, Wei-ting, Tutchton, Roxanne M., Resta, Giacomo, Lee, Tsung-Han, Bauer, Eric D., Ronning, Filip, Scalettar, Richard T., and Zhu, Jian-Xin. Hybridization effect on the x-ray absorption spectra for actinide materials: Application to PuB4. United States: N. p., 2020.
Web. doi:10.1103/physrevb.102.085150.
Chiu, Wei-ting, Tutchton, Roxanne M., Resta, Giacomo, Lee, Tsung-Han, Bauer, Eric D., Ronning, Filip, Scalettar, Richard T., & Zhu, Jian-Xin. Hybridization effect on the x-ray absorption spectra for actinide materials: Application to PuB4. United States. https://doi.org/10.1103/physrevb.102.085150
Chiu, Wei-ting, Tutchton, Roxanne M., Resta, Giacomo, Lee, Tsung-Han, Bauer, Eric D., Ronning, Filip, Scalettar, Richard T., and Zhu, Jian-Xin. Wed .
"Hybridization effect on the x-ray absorption spectra for actinide materials: Application to PuB4". United States. https://doi.org/10.1103/physrevb.102.085150. https://www.osti.gov/servlets/purl/1726189.
@article{osti_1726189,
title = {Hybridization effect on the x-ray absorption spectra for actinide materials: Application to PuB4},
author = {Chiu, Wei-ting and Tutchton, Roxanne M. and Resta, Giacomo and Lee, Tsung-Han and Bauer, Eric D. and Ronning, Filip and Scalettar, Richard T. and Zhu, Jian-Xin},
abstractNote = {Studying the local moment and 5f-electron occupations sheds insight into the electronic behavior in actinide materials. X-ray absorption spectroscopy (XAS) has been a powerful tool to reveal the valence electronic structure when assisted with theoretical calculations. However, the analysis currently taken in the community on the branching ratio of the XAS spectra generally does not account for the hybridization effects between local f orbitals and conduction states. In this paper, we discuss an approach which employs the density functional theory plus Gutzwiller rotationally invariant slave boson method to obtain a local Hamiltonian for the single-impurity Anderson model, and calculates the XAS spectra by the exact diagonalization (ED) method. A customized numerical routine was implemented for the ED XAS part of the calculation. By applying this technique to the recently discovered 5f-electron topological Kondo insulator PuB4, we determined the signature of 5f-electronic correlation effects in the theoretical x-ray spectra. Furthermore, we found that the Pu 5f-6d hybridization effect provides an extra channel to mix the j=5/2 and 7/2 orbitals in the 5f valence. As a consequence, the resulting electron occupation number and spin-orbit coupling strength deviate from the intermediate-coupling regime.},
doi = {10.1103/physrevb.102.085150},
journal = {Physical Review B},
number = 8,
volume = 102,
place = {United States},
year = {Wed Aug 26 00:00:00 EDT 2020},
month = {Wed Aug 26 00:00:00 EDT 2020}
}
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