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Title: Electrostatic potential and valence modulation in La 0.7Sr 0.3MnO 3 thin films

Abstract

The Mn valence in thin film La 0.7Sr 0.3MnO 3 was studied as a function of film thickness in the range of 1–16 unit cells with a combination of non-destructive bulk and surface sensitive X-ray absorption spectroscopy techniques. Using a layer-by-layer valence model, it was found that while the bulk averaged valence hovers around its expected value of 3.3, a significant deviation occurs within several unit cells of the surface and interface. These results were supported by first principles calculations. The surface valence increases to up to Mn 3.7+, whereas the interface valence reduces down to Mn 2.5+. The change in valence from the expected bulk value is consistent with charge redistribution due to the polar discontinuity at the film-substrate interface. The comparison with theory employed here illustrates how this layer-by-layer valence evolves with film thickness and allows for a deeper understanding of the microscopic mechanisms at play in this effect. These results offer insight on how the two-dimensional electron gas is created in thin film oxide alloys and how the magnetic ordering is reduced with dimensionality.

Authors:
ORCiD logo [1];  [2];  [3];  [4];  [5];  [6]; ORCiD logo [1];  [1];  [1];  [3];  [6]; ORCiD logo [5]; ORCiD logo [1]
  1. West Virginia Univ., Morgantown, WV (United States). Dept. of Physics and Astronomy
  2. West Virginia Univ., Morgantown, WV (United States). Dept. of Physics and Astronomy; Univ. of Liège (Belgium). Theoretical Physics of Materials; Industrial Univ. of Santander, Bucaramanga (Colombia). Dept. of Physics
  3. National Chiao Tung Univ., Hsinchu (Taiwan). Inst. of Physics
  4. West Virginia Univ., Morgantown, WV (United States). Dept. of Mechanical & Aerospace Engineering
  5. West Virginia Univ., Morgantown, WV (United States). Dept. of Physics and Astronomy; Meritorious Autonomous Univ. of Puebla (BUAP) (Mexico). Faculty of Engineering
  6. North Carolina State Univ., Raleigh, NC (United States). Dept. of Materials Science and Engineering
Publication Date:
Research Org.:
West Virginia Univ., Morgantown, WV (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
OSTI Identifier:
1499989
Grant/Contract Number:  
SC0016176; AC02-05CH11231; DMR-1608656; ACI-1053575; DMREF-NSF 1434897
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; electronic properties and materials; surfaces; interfaces and thin films

Citation Formats

Trappen, Robbyn, Garcia-Castro, A. C., Tra, Vu Thanh, Huang, Chih-Yeh, Ibarra-Hernandez, Wilfredo, Fitch, James, Singh, Sobhit, Zhou, Jinling, Cabrera, Guerau, Chu, Ying-Hao, LeBeau, James M., Romero, Aldo H., and Holcomb, Mikel B. Electrostatic potential and valence modulation in La0.7Sr0.3MnO3 thin films. United States: N. p., 2018. Web. doi:10.1038/s41598-018-32701-x.
Trappen, Robbyn, Garcia-Castro, A. C., Tra, Vu Thanh, Huang, Chih-Yeh, Ibarra-Hernandez, Wilfredo, Fitch, James, Singh, Sobhit, Zhou, Jinling, Cabrera, Guerau, Chu, Ying-Hao, LeBeau, James M., Romero, Aldo H., & Holcomb, Mikel B. Electrostatic potential and valence modulation in La0.7Sr0.3MnO3 thin films. United States. doi:10.1038/s41598-018-32701-x.
Trappen, Robbyn, Garcia-Castro, A. C., Tra, Vu Thanh, Huang, Chih-Yeh, Ibarra-Hernandez, Wilfredo, Fitch, James, Singh, Sobhit, Zhou, Jinling, Cabrera, Guerau, Chu, Ying-Hao, LeBeau, James M., Romero, Aldo H., and Holcomb, Mikel B. Tue . "Electrostatic potential and valence modulation in La0.7Sr0.3MnO3 thin films". United States. doi:10.1038/s41598-018-32701-x. https://www.osti.gov/servlets/purl/1499989.
@article{osti_1499989,
title = {Electrostatic potential and valence modulation in La0.7Sr0.3MnO3 thin films},
author = {Trappen, Robbyn and Garcia-Castro, A. C. and Tra, Vu Thanh and Huang, Chih-Yeh and Ibarra-Hernandez, Wilfredo and Fitch, James and Singh, Sobhit and Zhou, Jinling and Cabrera, Guerau and Chu, Ying-Hao and LeBeau, James M. and Romero, Aldo H. and Holcomb, Mikel B.},
abstractNote = {The Mn valence in thin film La0.7Sr0.3MnO3 was studied as a function of film thickness in the range of 1–16 unit cells with a combination of non-destructive bulk and surface sensitive X-ray absorption spectroscopy techniques. Using a layer-by-layer valence model, it was found that while the bulk averaged valence hovers around its expected value of 3.3, a significant deviation occurs within several unit cells of the surface and interface. These results were supported by first principles calculations. The surface valence increases to up to Mn3.7+, whereas the interface valence reduces down to Mn2.5+. The change in valence from the expected bulk value is consistent with charge redistribution due to the polar discontinuity at the film-substrate interface. The comparison with theory employed here illustrates how this layer-by-layer valence evolves with film thickness and allows for a deeper understanding of the microscopic mechanisms at play in this effect. These results offer insight on how the two-dimensional electron gas is created in thin film oxide alloys and how the magnetic ordering is reduced with dimensionality.},
doi = {10.1038/s41598-018-32701-x},
journal = {Scientific Reports},
number = ,
volume = 8,
place = {United States},
year = {2018},
month = {9}
}

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Figures / Tables:

Figure 1 Figure 1: (a) TEM image of the film-substrate interface. (b) Results of the linear combination fits for the Mn K and L-edges. (c) Valence obtained from the linear combination fits (solid points) and experimental fit using the layer dependent valence model (solid lines). The dashed line indicates the expected bulkmore » Mn valence of 3.3.« less

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    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.