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Title: Depth-Resolved Modulation of Metal-Oxygen Hybridization and Orbital Polarization across Correlated Oxide Interfaces

Abstract

Interface-induced modifications of the electronic, magnetic, and lattice degrees of freedom drive an array of novel physical properties in oxide heterostructures. Here large changes in metal-oxygen band hybridization, as measured in the oxygen ligand hole density, are induced as a result of interfacing two isovalent correlated oxides. Using resonant x-ray reflectivity, a superlattice of SrFeO3 and CaFeO3 is shown to exhibit an electronic character that spatially evolves from strongly O-like in SrFeO3 to strongly Fe-like in CaFeO3. This alternating degree of Fe electronic character is correlated with a modulation of an Fe 3d orbital polarization, giving rise to an orbital superstructure. At the SrFeO3/CaFeO3 interfaces, the ligand hole density and orbital polarization reconstruct in a single unit cell of CaFeO3, demonstrating how the mismatch in these electronic parameters is accommodated at the interface. These results provide new insight into how the orbital character of electrons is altered by correlated oxide interfaces and lays out a broadly applicable approach for depth-resolving band hybridization.

Authors:
 [1];  [2];  [3];  [4];  [2];  [5];  [3];  [6]; ORCiD logo [1]
+ Show Author Affiliations
  1. Drexel Univ., Philadelphia, PA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Condensed Matter Physics and Materials Science Dept.
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
  5. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  6. Univ. of British Columbia, Vancouver, BC (Canada); Univ. of Saskatchewan, Saskatoon, SK (Canada)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Army Research Office (ARO)
OSTI Identifier:
1570671
Alternate Identifier(s):
OSTI ID: 1561563; OSTI ID: 1756864
Report Number(s):
BNL-212192-2019-JAAM
Journal ID: ISSN 0935-9648
Grant/Contract Number:  
SC0012704; AC02‐05CH11231; AC02‐06CH11357; W911NF‐14‐1‐0493; W911NF‐15‐1‐0133; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 31; Journal Issue: 43; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Band hybridization; oxide interfaces; resonant X‐ray reflectivity; transition metal oxides; band hybridization; resonant x-ray reflectivity

Citation Formats

Rogge, Paul C., Shafer, Padraic, Fabbris, Gilberto, Hu, Wen, Arenholz, Elke, Karapetrova, Evguenia, Dean, Mark P. M., Green, Robert J., and May, Steven J. Depth-Resolved Modulation of Metal-Oxygen Hybridization and Orbital Polarization across Correlated Oxide Interfaces. United States: N. p., 2019. Web. doi:10.1002/adma.201902364.
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Rogge, Paul C., Shafer, Padraic, Fabbris, Gilberto, Hu, Wen, Arenholz, Elke, Karapetrova, Evguenia, Dean, Mark P. M., Green, Robert J., & May, Steven J. Depth-Resolved Modulation of Metal-Oxygen Hybridization and Orbital Polarization across Correlated Oxide Interfaces. United States. https://doi.org/10.1002/adma.201902364
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Rogge, Paul C., Shafer, Padraic, Fabbris, Gilberto, Hu, Wen, Arenholz, Elke, Karapetrova, Evguenia, Dean, Mark P. M., Green, Robert J., and May, Steven J. Thu . "Depth-Resolved Modulation of Metal-Oxygen Hybridization and Orbital Polarization across Correlated Oxide Interfaces". United States. https://doi.org/10.1002/adma.201902364. https://www.osti.gov/servlets/purl/1570671.
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@article{osti_1570671,
title = {Depth-Resolved Modulation of Metal-Oxygen Hybridization and Orbital Polarization across Correlated Oxide Interfaces},
author = {Rogge, Paul C. and Shafer, Padraic and Fabbris, Gilberto and Hu, Wen and Arenholz, Elke and Karapetrova, Evguenia and Dean, Mark P. M. and Green, Robert J. and May, Steven J.},
abstractNote = {Interface-induced modifications of the electronic, magnetic, and lattice degrees of freedom drive an array of novel physical properties in oxide heterostructures. Here large changes in metal-oxygen band hybridization, as measured in the oxygen ligand hole density, are induced as a result of interfacing two isovalent correlated oxides. Using resonant x-ray reflectivity, a superlattice of SrFeO3 and CaFeO3 is shown to exhibit an electronic character that spatially evolves from strongly O-like in SrFeO3 to strongly Fe-like in CaFeO3. This alternating degree of Fe electronic character is correlated with a modulation of an Fe 3d orbital polarization, giving rise to an orbital superstructure. At the SrFeO3/CaFeO3 interfaces, the ligand hole density and orbital polarization reconstruct in a single unit cell of CaFeO3, demonstrating how the mismatch in these electronic parameters is accommodated at the interface. These results provide new insight into how the orbital character of electrons is altered by correlated oxide interfaces and lays out a broadly applicable approach for depth-resolving band hybridization.},
doi = {10.1002/adma.201902364},
journal = {Advanced Materials},
number = 43,
volume = 31,
place = {United States},
year = {Thu Sep 12 00:00:00 EDT 2019},
month = {Thu Sep 12 00:00:00 EDT 2019}
}
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Journal Article:
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https://doi.org/10.1002/adma.201902364
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