Inverted orbital polarization in strained correlated oxide films

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.

doi:10.1103/PhysRevB.98.201115

Inverted orbital polarization in strained correlated oxide films

Journal Article · Wed Nov 28 00:00:00 EST 2018 · Physical Review. B

DOI:https://doi.org/10.1103/PhysRevB.98.201115· OSTI ID:1480920

Rogge, Paul C. ^[1]; Green, Robert J. ^[2]; Shafer, Padraic ^[3]; Fabbris, Gilberto ^[4]; Barbour, Andi M. ^[5]; Lefler, Benjamin M. ^[1]; Arenholz, Elke ^[3]; Dean, Mark P. M. ^[4]; May, Steven J. ^[1]

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)

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 con rmed 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. Here, 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 new method to engineer otherwise unachievable orbital occupations in correlated oxides.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: US Army Research Office (ARO); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-05CH11231; SC0012704

OSTI ID:: 1480920

Alternate ID(s):: OSTI ID: 1580343
OSTI ID: 1483722

Report Number(s):: BNL--209416-2018-JAAM

Journal Information:: Physical Review. B, Journal Name: Physical Review. B Journal Issue: 20 Vol. 98; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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