Inverted orbital polarization in strained correlated oxide films
Abstract
© 2018 American Physical Society. Manipulating the orbital occupation of valence electrons via epitaxial strain in an effort to induce new functional properties requires considerations of how changes in the local bonding environment affect the band structure at the Fermi level. Using synchrotron radiation to measure the x-ray linear dichroism of epitaxially strained films of the correlated oxide CaFeO3, we demonstrate that the orbital polarization of the Fe valence electrons is opposite from conventional understanding. Although the energetic ordering of the Fe 3d orbitals is confirmed by multiplet ligand field theory analysis to be consistent with previously reported strain-induced behavior, we find that the nominally higher energy orbital is more populated than the lower. We ascribe this inverted orbital polarization to an anisotropic bandwidth response to strain in a compound with nearly filled bands. These findings provide an important counterexample to the traditional understanding of strain-induced orbital polarization and reveal a method to engineer otherwise unachievable orbital occupations in correlated oxides.
- Authors:
-
- Drexel Univ., Philadelphia, PA (United States). Dept. of Materials Science and Engineering
- Univ. of British Columbia, Vancouver, BC (Canada). Stewart Blusson Quantum Matter Inst.; Univ. of Saskatchewan, Saskatoon, Saskatchewan (Canada). Dept. of Physics and Engineering Physics
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
- Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Condensed Matter Physics and Materials Science
- Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); US Army Research Office (ARO)
- OSTI Identifier:
- 1480920
- Alternate Identifier(s):
- OSTI ID: 1483722; OSTI ID: 1580343
- Report Number(s):
- BNL-209416-2018-JAAM
Journal ID: ISSN 2469-9950
- Grant/Contract Number:
- SC0012704; W911NF-15-1-0133; W911NF-14-1-0493; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review. B
- Additional Journal Information:
- Journal Volume: 98; Journal Issue: 20; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY
Citation Formats
Rogge, Paul C., Green, Robert J., Shafer, Padraic, Fabbris, Gilberto, Barbour, Andi M., Lefler, Benjamin M., Arenholz, Elke, Dean, Mark P. M., and May, Steven J. Inverted orbital polarization in strained correlated oxide films. United States: N. p., 2018.
Web. doi:10.1103/PhysRevB.98.201115.
Rogge, Paul C., Green, Robert J., Shafer, Padraic, Fabbris, Gilberto, Barbour, Andi M., Lefler, Benjamin M., Arenholz, Elke, Dean, Mark P. M., & May, Steven J. Inverted orbital polarization in strained correlated oxide films. United States. https://doi.org/10.1103/PhysRevB.98.201115
Rogge, Paul C., Green, Robert J., Shafer, Padraic, Fabbris, Gilberto, Barbour, Andi M., Lefler, Benjamin M., Arenholz, Elke, Dean, Mark P. M., and May, Steven J. Wed .
"Inverted orbital polarization in strained correlated oxide films". United States. https://doi.org/10.1103/PhysRevB.98.201115. https://www.osti.gov/servlets/purl/1480920.
@article{osti_1480920,
title = {Inverted orbital polarization in strained correlated oxide films},
author = {Rogge, Paul C. and Green, Robert J. and Shafer, Padraic and Fabbris, Gilberto and Barbour, Andi M. and Lefler, Benjamin M. and Arenholz, Elke and Dean, Mark P. M. and May, Steven J.},
abstractNote = {© 2018 American Physical Society. Manipulating the orbital occupation of valence electrons via epitaxial strain in an effort to induce new functional properties requires considerations of how changes in the local bonding environment affect the band structure at the Fermi level. Using synchrotron radiation to measure the x-ray linear dichroism of epitaxially strained films of the correlated oxide CaFeO3, we demonstrate that the orbital polarization of the Fe valence electrons is opposite from conventional understanding. Although the energetic ordering of the Fe 3d orbitals is confirmed by multiplet ligand field theory analysis to be consistent with previously reported strain-induced behavior, we find that the nominally higher energy orbital is more populated than the lower. We ascribe this inverted orbital polarization to an anisotropic bandwidth response to strain in a compound with nearly filled bands. These findings provide an important counterexample to the traditional understanding of strain-induced orbital polarization and reveal a method to engineer otherwise unachievable orbital occupations in correlated oxides.},
doi = {10.1103/PhysRevB.98.201115},
journal = {Physical Review. B},
number = 20,
volume = 98,
place = {United States},
year = {Wed Nov 28 00:00:00 EST 2018},
month = {Wed Nov 28 00:00:00 EST 2018}
}
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Works referencing / citing this record:
Depth‐Resolved Modulation of Metal–Oxygen Hybridization and Orbital Polarization across Correlated Oxide Interfaces
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