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Title: Electronic structure of lanthanide scandates

Here, x-ray photoelectron spectroscopy, ultraviolet photoelectron spectroscopy, and density functional theory calculations were used to study the electronic structure of three lanthanide scandates: GdScO3, TbScO3, and DyScO3. X-ray photoelectron spectra simulated from first-principles calculations using a combination of on-site hybrid and GGA + U methods were found to be in good agreement with experimental x-ray photoelectron spectra. The hybrid method was used to model the ground state electronic structure and the GGA + U method accounted for the shift of valence state energies due to photoelectron emission via a Slater-Janak transition state approach. From these results, the lanthanide scandate valence bands were determined to be composed of Ln4f, O2p, and Sc3d states, in agreement with previous work. However, contrary to previous work the minority Ln4f states were found to be located closer to, and in some cases at, the valence band maximum. This suggests that minority Ln4f electrons may play a larger role in lanthanide scandate properties than previously thought.
Authors:
 [1] ;  [1] ;  [1]
  1. Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
Publication Date:
Grant/Contract Number:
FG02-01ER45945
Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 2; Journal Issue: 2; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Research Org:
Northwestern Univ., Evanston, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 74 ATOMIC AND MOLECULAR PHYSICS; density of states; electronic structure; insulators; oxides; strongly correlated systems; density functional theory; x-ray photoelectron spectroscopy
OSTI Identifier:
1469191
Alternate Identifier(s):
OSTI ID: 1421303

Mizzi, Christopher A., Koirala, Pratik, and Marks, Laurence D.. Electronic structure of lanthanide scandates. United States: N. p., Web. doi:10.1103/PhysRevMaterials.2.025001.
Mizzi, Christopher A., Koirala, Pratik, & Marks, Laurence D.. Electronic structure of lanthanide scandates. United States. doi:10.1103/PhysRevMaterials.2.025001.
Mizzi, Christopher A., Koirala, Pratik, and Marks, Laurence D.. 2018. "Electronic structure of lanthanide scandates". United States. doi:10.1103/PhysRevMaterials.2.025001.
@article{osti_1469191,
title = {Electronic structure of lanthanide scandates},
author = {Mizzi, Christopher A. and Koirala, Pratik and Marks, Laurence D.},
abstractNote = {Here, x-ray photoelectron spectroscopy, ultraviolet photoelectron spectroscopy, and density functional theory calculations were used to study the electronic structure of three lanthanide scandates: GdScO3, TbScO3, and DyScO3. X-ray photoelectron spectra simulated from first-principles calculations using a combination of on-site hybrid and GGA + U methods were found to be in good agreement with experimental x-ray photoelectron spectra. The hybrid method was used to model the ground state electronic structure and the GGA + U method accounted for the shift of valence state energies due to photoelectron emission via a Slater-Janak transition state approach. From these results, the lanthanide scandate valence bands were determined to be composed of Ln4f, O2p, and Sc3d states, in agreement with previous work. However, contrary to previous work the minority Ln4f states were found to be located closer to, and in some cases at, the valence band maximum. This suggests that minority Ln4f electrons may play a larger role in lanthanide scandate properties than previously thought.},
doi = {10.1103/PhysRevMaterials.2.025001},
journal = {Physical Review Materials},
number = 2,
volume = 2,
place = {United States},
year = {2018},
month = {2}
}

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