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Title: Modified Oxygen Defect Chemistry at Transition Metal Oxide Heterostructures Probed by Hard X-ray Photoelectron Spectroscopy and X-ray Diffraction

Transition metal oxide hetero-structures are interesting due to the distinctly different properties that can arise from their interfaces, such as superconductivity, high catalytic activity and magnetism. Oxygen point defects can play an important role at these interfaces in inducing potentially novel properties. The design of oxide hetero-structures in which the oxygen defects are manipulated to attain specific functionalities requires the ability to resolve the state and concentration of local oxygen defects across buried interfaces. In this work, we utilized a novel combination of hard x-ray photoelectron spectroscopy (HAXPES) and high resolution xray diffraction (HRXRD) to probe the local oxygen defect distribution across the buried interfaces of oxide heterolayers. This approach provides a non-destructive way to qualitatively probe locally the oxygen defects in transition metal oxide hetero-structures. We studied two trilayer structures as model systems - the La 0.8Sr 0.2CoO 3-δ/(La 0.5Sr 0.5) 2CoO 4/La 0.8Sr 0.2CoO 3-δ (LSC 113/LSC 214) and the La 0.8Sr 0.2CoO 3-δ/La 2NiO 4+δ/La 0.8Sr 0.2CoO 3-δ (LSC 113/LNO 214) on SrTiO 3(001) single crystal substrates. We found that the oxygen defect chemistry of these transition metal oxides was strongly impacted by the presence of interfaces and the properties of the adjacent phases. Under reducing conditions,more » the LSC 113 in the LSC 113/LNO 214 tri-layer had less oxygen vacancies than the LSC 113 in the LSC 113/LSC 214 tri-layer and the LSC 113 single phase film. On the other hand, LSC 214 and LNO 214 were more reduced in the two tri-layer structures when in contact with the LSC 113 layer compared to their single phase counterparts. Furthermore, the results point out a potential way to modify the local oxygen defect states at oxide hetero-interfaces.« less
Authors:
ORCiD logo [1] ;  [2] ;  [1] ;  [3] ;  [4] ;  [1] ;  [1]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
  3. Synchrotron SOLEIL, Saint-Aubin (France)
  4. Synchrotron SOLEIL, Saint-Aubin (France); Sorbonne Univ., Paris (France)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 30; Journal Issue: 10; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
OSTI Identifier:
1455048

Chen, Yan, Fong, Dillon D., Herbert, F. William, Rault, Julien, Rueff, Jean -Pascal, Tsvetkov, Nikolai, and Yildiz, Bilge. Modified Oxygen Defect Chemistry at Transition Metal Oxide Heterostructures Probed by Hard X-ray Photoelectron Spectroscopy and X-ray Diffraction. United States: N. p., Web. doi:10.1021/acs.chemmater.8b00808.
Chen, Yan, Fong, Dillon D., Herbert, F. William, Rault, Julien, Rueff, Jean -Pascal, Tsvetkov, Nikolai, & Yildiz, Bilge. Modified Oxygen Defect Chemistry at Transition Metal Oxide Heterostructures Probed by Hard X-ray Photoelectron Spectroscopy and X-ray Diffraction. United States. doi:10.1021/acs.chemmater.8b00808.
Chen, Yan, Fong, Dillon D., Herbert, F. William, Rault, Julien, Rueff, Jean -Pascal, Tsvetkov, Nikolai, and Yildiz, Bilge. 2018. "Modified Oxygen Defect Chemistry at Transition Metal Oxide Heterostructures Probed by Hard X-ray Photoelectron Spectroscopy and X-ray Diffraction". United States. doi:10.1021/acs.chemmater.8b00808.
@article{osti_1455048,
title = {Modified Oxygen Defect Chemistry at Transition Metal Oxide Heterostructures Probed by Hard X-ray Photoelectron Spectroscopy and X-ray Diffraction},
author = {Chen, Yan and Fong, Dillon D. and Herbert, F. William and Rault, Julien and Rueff, Jean -Pascal and Tsvetkov, Nikolai and Yildiz, Bilge},
abstractNote = {Transition metal oxide hetero-structures are interesting due to the distinctly different properties that can arise from their interfaces, such as superconductivity, high catalytic activity and magnetism. Oxygen point defects can play an important role at these interfaces in inducing potentially novel properties. The design of oxide hetero-structures in which the oxygen defects are manipulated to attain specific functionalities requires the ability to resolve the state and concentration of local oxygen defects across buried interfaces. In this work, we utilized a novel combination of hard x-ray photoelectron spectroscopy (HAXPES) and high resolution xray diffraction (HRXRD) to probe the local oxygen defect distribution across the buried interfaces of oxide heterolayers. This approach provides a non-destructive way to qualitatively probe locally the oxygen defects in transition metal oxide hetero-structures. We studied two trilayer structures as model systems - the La0.8Sr0.2CoO3-δ/(La0.5Sr0.5)2CoO4/La0.8Sr0.2CoO3-δ (LSC113/LSC214) and the La0.8Sr0.2CoO3-δ/La2NiO4+δ/La0.8Sr0.2CoO3-δ (LSC113/LNO214) on SrTiO3(001) single crystal substrates. We found that the oxygen defect chemistry of these transition metal oxides was strongly impacted by the presence of interfaces and the properties of the adjacent phases. Under reducing conditions, the LSC113 in the LSC113/LNO214 tri-layer had less oxygen vacancies than the LSC113 in the LSC113/LSC214 tri-layer and the LSC113 single phase film. On the other hand, LSC214 and LNO214 were more reduced in the two tri-layer structures when in contact with the LSC113 layer compared to their single phase counterparts. Furthermore, the results point out a potential way to modify the local oxygen defect states at oxide hetero-interfaces.},
doi = {10.1021/acs.chemmater.8b00808},
journal = {Chemistry of Materials},
number = 10,
volume = 30,
place = {United States},
year = {2018},
month = {4}
}