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Title: Two-dimensional electron systems in perovskite oxide heterostructures: Role of the polarity-induced substitutional defects

Abstract

The discovery of a two-dimensional electron system (2DES) at the interfaces of perovskite oxides such as LaAlO3 and SrTiO3 has motivated enormous efforts in engineering interfacial functionalities with this type of oxide heterostructures. However, the fundamental origins of the 2DES are still not understood, e.g., the microscopic mechanisms of coexisting interface conductivity and magnetism. In this paper, we report a comprehensive spectroscopic investigation on the depth profile of 2DES-relevant Ti 3d interface carriers using depth- and element-specific techniques like standing-wave excited photoemission and resonant inelastic scattering. We found that one type of Ti 3d interface carriers, which give rise to the 2DES are located within three unit cells from the n-type interface in the SrTiO3 layer. Unexpectedly, another type of interface carriers, which are polarity-induced Ti-on-Al antisite defects, reside in the first three unit cells of the opposing LaAlO3 layer (~10 Å). Our findings provide a microscopic picture of how the localized and mobile Ti 3d interface carriers distribute across the interface and suggest that the 2DES and 2D magnetism at the LaAlO3/SrTiO3 interface have disparate explanations as originating from different types of interface carriers.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [4];  [5];  [6];  [1]; ORCiD logo [7];  [3]; ORCiD logo [3];  [8]; ORCiD logo [3]; ORCiD logo [9];  [10];  [11];  [7];  [12];  [1]
  1. Univ. of California, Davis, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Univ. of California, Davis, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  4. Univ. of Twente, Enschede (Netherlands)
  5. Synchrotron SOLEIL, Gif-sur-Yvette (France); Sorbonne Univ., Paris (France). CNRS Lab. de Chimie Physique-Matiere et Rayonnement
  6. Federal Univ. of Parana, Curitiba (Brazil)
  7. Politecnico di Milano (Italy)
  8. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  9. Stanford Univ., CA (United States). Stanford Nano Shared Facilities; Kaunas Univ. of Technology (Lithuania)
  10. Univ. of Twente, Enschede (Netherlands); Univ. of Antwerp (Belgium). Electron Microscopy for Materials Science (EMAT)
  11. Univ. of Antwerp (Belgium). Electron Microscopy for Materials Science (EMAT)
  12. Univ. of California, Davis, CA (United States); Forschungszentrum Juulich (Germany). Peter Grunberg Inst. PGI-6
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); European Union Horizon 2020; Brazilian National Council for Scientific and Technological Development (CNPq); Coordination for the Improvement of Higher Education Personnel (CAPES); Flemish Government
OSTI Identifier:
1762200
Alternate Identifier(s):
OSTI ID: 1720173
Grant/Contract Number:  
AC02-05CH11231; SC0014697; 823717; n°823717
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 4; Journal Issue: 11; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; electronic structure; surface & interfacial phenomena; multilayer thin films; two-dimensional electron gas; hard x-ray photoelectron spectroscopy; resonant inelastic x-ray scattering; x-ray photoelectron spectroscopy; x-ray standing waves; two-dimensional electron system; perovskite oxide; x-ray standing wave

Citation Formats

Lin, Shih-Chieh, Kuo, Cheng-Tai, Shao, Yu-Cheng, Chuang, Yi-De, Geessinck, Jaap, Huijben, Mark, Rueff, Jean-Pascal, Graff, Ismael L., Conti, Giuseppina, Peng, Yingying, Bostwick, Aaron, Rotenberg, Eli, Gullikson, Eric, Nemšák, Slavomír, Vailionis, Arturas, Gauquelin, Nicolas, Verbeeck, Johan, Ghiringhelli, Giacomo, Schneider, Claus M., and Fadley, Charles S. Two-dimensional electron systems in perovskite oxide heterostructures: Role of the polarity-induced substitutional defects. United States: N. p., 2020. Web. doi:10.1103/physrevmaterials.4.115002.
Lin, Shih-Chieh, Kuo, Cheng-Tai, Shao, Yu-Cheng, Chuang, Yi-De, Geessinck, Jaap, Huijben, Mark, Rueff, Jean-Pascal, Graff, Ismael L., Conti, Giuseppina, Peng, Yingying, Bostwick, Aaron, Rotenberg, Eli, Gullikson, Eric, Nemšák, Slavomír, Vailionis, Arturas, Gauquelin, Nicolas, Verbeeck, Johan, Ghiringhelli, Giacomo, Schneider, Claus M., & Fadley, Charles S. Two-dimensional electron systems in perovskite oxide heterostructures: Role of the polarity-induced substitutional defects. United States. https://doi.org/10.1103/physrevmaterials.4.115002
Lin, Shih-Chieh, Kuo, Cheng-Tai, Shao, Yu-Cheng, Chuang, Yi-De, Geessinck, Jaap, Huijben, Mark, Rueff, Jean-Pascal, Graff, Ismael L., Conti, Giuseppina, Peng, Yingying, Bostwick, Aaron, Rotenberg, Eli, Gullikson, Eric, Nemšák, Slavomír, Vailionis, Arturas, Gauquelin, Nicolas, Verbeeck, Johan, Ghiringhelli, Giacomo, Schneider, Claus M., and Fadley, Charles S. Thu . "Two-dimensional electron systems in perovskite oxide heterostructures: Role of the polarity-induced substitutional defects". United States. https://doi.org/10.1103/physrevmaterials.4.115002. https://www.osti.gov/servlets/purl/1762200.
@article{osti_1762200,
title = {Two-dimensional electron systems in perovskite oxide heterostructures: Role of the polarity-induced substitutional defects},
author = {Lin, Shih-Chieh and Kuo, Cheng-Tai and Shao, Yu-Cheng and Chuang, Yi-De and Geessinck, Jaap and Huijben, Mark and Rueff, Jean-Pascal and Graff, Ismael L. and Conti, Giuseppina and Peng, Yingying and Bostwick, Aaron and Rotenberg, Eli and Gullikson, Eric and Nemšák, Slavomír and Vailionis, Arturas and Gauquelin, Nicolas and Verbeeck, Johan and Ghiringhelli, Giacomo and Schneider, Claus M. and Fadley, Charles S.},
abstractNote = {The discovery of a two-dimensional electron system (2DES) at the interfaces of perovskite oxides such as LaAlO3 and SrTiO3 has motivated enormous efforts in engineering interfacial functionalities with this type of oxide heterostructures. However, the fundamental origins of the 2DES are still not understood, e.g., the microscopic mechanisms of coexisting interface conductivity and magnetism. In this paper, we report a comprehensive spectroscopic investigation on the depth profile of 2DES-relevant Ti 3d interface carriers using depth- and element-specific techniques like standing-wave excited photoemission and resonant inelastic scattering. We found that one type of Ti 3d interface carriers, which give rise to the 2DES are located within three unit cells from the n-type interface in the SrTiO3 layer. Unexpectedly, another type of interface carriers, which are polarity-induced Ti-on-Al antisite defects, reside in the first three unit cells of the opposing LaAlO3 layer (~10 Å). Our findings provide a microscopic picture of how the localized and mobile Ti 3d interface carriers distribute across the interface and suggest that the 2DES and 2D magnetism at the LaAlO3/SrTiO3 interface have disparate explanations as originating from different types of interface carriers.},
doi = {10.1103/physrevmaterials.4.115002},
journal = {Physical Review Materials},
number = 11,
volume = 4,
place = {United States},
year = {Thu Nov 19 00:00:00 EST 2020},
month = {Thu Nov 19 00:00:00 EST 2020}
}

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