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:
-
- Univ. of California, Davis, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- 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)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
- Univ. of Twente, Enschede (Netherlands)
- Synchrotron SOLEIL, Gif-sur-Yvette (France); Sorbonne Univ., Paris (France). CNRS Lab. de Chimie Physique-Matiere et Rayonnement
- Federal Univ. of Parana, Curitiba (Brazil)
- Politecnico di Milano (Italy)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Stanford Univ., CA (United States). Stanford Nano Shared Facilities; Kaunas Univ. of Technology (Lithuania)
- Univ. of Twente, Enschede (Netherlands); Univ. of Antwerp (Belgium). Electron Microscopy for Materials Science (EMAT)
- Univ. of Antwerp (Belgium). Electron Microscopy for Materials Science (EMAT)
- 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}
}
Works referenced in this record:
Effects of structural relaxation, interdiffusion, and surface termination on two-dimensional electron gas formation at the (001) interface
journal, October 2015
- Fongkaew, Ittipon; Limpijumnnong, Sukit; Lambrecht, Walter R. L.
- Physical Review B, Vol. 92, Issue 15
Probing core-electron orbitals by scanning transmission electron microscopy and measuring the delocalization of core-level excitations
journal, April 2016
- Jeong, Jong Seok; Odlyzko, Michael L.; Xu, Peng
- Physical Review B, Vol. 93, Issue 16
Electronically coupled complementary interfaces between perovskite band insulators
journal, June 2006
- Huijben, Mark; Rijnders, Guus; Blank, Dave H. A.
- Nature Materials, Vol. 5, Issue 7
Structural Basis for the Conducting Interface between and
journal, October 2007
- Willmott, P. R.; Pauli, S. A.; Herger, R.
- Physical Review Letters, Vol. 99, Issue 15, Article No. 155502
Cation mixing, band offsets and electric fields at LaAlO3/SrTiO3(001) heterojunctions with variable La:Al atom ratio
journal, August 2011
- Qiao, L.; Droubay, T. C.; Kaspar, T. C.
- Surface Science, Vol. 605, Issue 15-16
Enhanced Local Magnetization by Interface Engineering in Perovskite-Type Correlated Oxide Heterostructures
journal, January 2015
- Huijben, Mark; Liu, Yaohua; Boschker, Hans
- Advanced Materials Interfaces, Vol. 2, Issue 3
Scattering delocalization and radiation damage in STEM-EELS
journal, September 2017
- Egerton, R. F.
- Ultramicroscopy, Vol. 180
Spectroscopic evidence of in-gap states at the SrTiO3/LaAlO3 ultrathin interfaces
journal, January 2011
- Drera, G.; Banfi, F.; Canova, F. Federici
- Applied Physics Letters, Vol. 98, Issue 5
oxide heterostructures studied by resonant inelastic x-ray scattering
journal, December 2010
- Berner, G.; Glawion, S.; Walde, J.
- Physical Review B, Vol. 82, Issue 24
Suppression of Near-Fermi Level Electronic States at the Interface in a Superlattice
journal, September 2011
- Kaiser, A. M.; Gray, A. X.; Conti, G.
- Physical Review Letters, Vol. 107, Issue 11
Future directions in standing-wave photoemission
journal, August 2014
- Gray, Alexander X.
- Journal of Electron Spectroscopy and Related Phenomena, Vol. 195
Profiling the Interface Electron Gas of Heterostructures with Hard X-Ray Photoelectron Spectroscopy
journal, April 2009
- Sing, M.; Berner, G.; Goß, K.
- Physical Review Letters, Vol. 102, Issue 17
Electronic phase separation at interfaces tunable by oxygen deficiency
journal, October 2019
- Strocov, V. N.; Chikina, A.; Caputo, M.
- Physical Review Materials, Vol. 3, Issue 10
Depth-resolved resonant inelastic x-ray scattering at a superconductor/half-metallic-ferromagnet interface through standing wave excitation
journal, December 2018
- Kuo, Cheng-Tai; Lin, Shih-Chieh; Ghiringhelli, Giacomo
- Physical Review B, Vol. 98, Issue 23
Conducting channel at the LaAlO /SrTiO interface
journal, October 2013
- Huang, Z.; Wang, X. Renshaw; Liu, Z. Q.
- Physical Review B, Vol. 88, Issue 16
Localized and delocalized Ti 3 carriers in LaAlO /SrTiO superlattices revealed by resonant inelastic x-ray scattering
journal, May 2011
- Zhou, Ke-Jin; Radovic, Milan; Schlappa, Justine
- Physical Review B, Vol. 83, Issue 20
In-gap electronic structure of LaAlO -SrTiO heterointerfaces investigated by soft x-ray spectroscopy
journal, December 2011
- Koitzsch, A.; Ocker, J.; Knupfer, M.
- Physical Review B, Vol. 84, Issue 24
Mapping Band Alignment across Complex Oxide Heterointerfaces
journal, December 2012
- Huang, Bo-Chao; Chiu, Ya-Ping; Huang, Po-Cheng
- Physical Review Letters, Vol. 109, Issue 24
Orbital Ordering of the Mobile and Localized Electrons at Oxygen-Deficient LaAlO 3 /SrTiO 3 Interfaces
journal, July 2018
- Chikina, Alla; Lechermann, Frank; Husanu, Marius-Adrian
- ACS Nano, Vol. 12, Issue 8
Evolution of the SrTiO 3 surface electronic state as a function of LaAlO 3 overlayer thickness
journal, August 2017
- Plumb, N. C.; Kobayashi, M.; Salluzzo, M.
- Applied Surface Science, Vol. 412
Orbital Reconstruction and the Two-Dimensional Electron Gas at the Interface
journal, April 2009
- Salluzzo, M.; Cezar, J. C.; Brookes, N. B.
- Physical Review Letters, Vol. 102, Issue 16, Article No. 166804
Parallel Electron-Hole Bilayer Conductivity from Electronic Interface Reconstruction
journal, April 2010
- Pentcheva, R.; Huijben, M.; Otte, K.
- Physical Review Letters, Vol. 104, Issue 16
Two-dimensional electron gas with universal subbands at the surface of SrTiO3
journal, January 2011
- Santander-Syro, A. F.; Copie, O.; Kondo, T.
- Nature, Vol. 469, Issue 7329, p. 189-193
Control of orbital reconstruction in (LaAlO3)M/(SrTiO3)N(001) quantum wells by strain and confinement
journal, January 2015
- Doennig, David; Pentcheva, Rossitza
- Scientific Reports, Vol. 5, Issue 1
Interface properties and built-in potential profile of a superlattice determined by standing-wave excited photoemission spectroscopy
journal, October 2018
- Lin, S. -C.; Kuo, C. -T.; Comes, R. B.
- Physical Review B, Vol. 98, Issue 16
Magnetic effects at the interface between non-magnetic oxides
journal, June 2007
- Brinkman, A.; Huijben, M.; van Zalk, M.
- Nature Materials, Vol. 6, Issue 7, p. 493-496
Mapping the spatial distribution of charge carriers in LaAlO3/SrTiO3 heterostructures
journal, June 2008
- Basletic, M.; Maurice, J. -L.; Carrétéro, C.
- Nature Materials, Vol. 7, Issue 8
Real-space mapping of electronic orbitals
journal, June 2017
- Löffler, Stefan; Bugnet, Matthieu; Gauquelin, Nicolas
- Ultramicroscopy, Vol. 177
Defect Engineering in Oxide Heterostructures by Enhanced Oxygen Surface Exchange
journal, June 2013
- Huijben, Mark; Koster, Gertjan; Kruize, Michelle K.
- Advanced Functional Materials, Vol. 23, Issue 42
High Mobility in Heterostructures: Origin, Dimensionality, and Perspectives
journal, May 2007
- Herranz, G.; Basletić, M.; Bibes, M.
- Physical Review Letters, Vol. 98, Issue 21, Article No. 216803
Hard x-ray standing-wave photoemission insights into the structure of an epitaxial Fe/MgO multilayer magnetic tunnel junction
journal, August 2019
- Conlon, C. S.; Conti, G.; Nemšák, S.
- Journal of Applied Physics, Vol. 126, Issue 7
Modified spin relaxation mechanism by tunable coupling between interfacial two-dimensional electron gases in correlated oxide heterostructures
journal, August 2017
- Huijben, M.; Hassink, G. W. J.; Stehno, M. P.
- Physical Review B, Vol. 96, Issue 7
Hidden lattice instabilities as origin of the conductive interface between insulating LaAlO3 and SrTiO3
journal, September 2016
- Lee, P. W.; Singh, V. N.; Guo, G. Y.
- Nature Communications, Vol. 7, Issue 1
Carrier-Density Control of the SrTiO 3 (001) Surface 2D Electron Gas studied by ARPES
journal, May 2015
- Walker, Siobhan McKeown; Bruno, Flavio Yair; Wang, Zhiming
- Advanced Materials, Vol. 27, Issue 26
Limit of the electrostatic doping in two-dimensional electron gases of LaXO3(X = Al, Ti)/SrTiO3
journal, October 2014
- Biscaras, J.; Hurand, S.; Feuillet-Palma, C.
- Scientific Reports, Vol. 4, Issue 1
Making use of x-ray optical effects in photoelectron-, Auger electron-, and x-ray emission spectroscopies: Total reflection, standing-wave excitation, and resonant effects
journal, February 2013
- Yang, S. -H.; Gray, A. X.; Kaiser, A. M.
- Journal of Applied Physics, Vol. 113, Issue 7
Interface properties of magnetic tunnel junction superlattices studied by standing-wave excited photoemission spectroscopy
journal, November 2010
- Gray, A. X.; Papp, C.; Balke, B.
- Physical Review B, Vol. 82, Issue 20
Structure-Property Relation of SrTiO3/LaAlO3 Interfaces
journal, May 2009
- Huijben, Mark; Brinkman, Alexander; Koster, Gertjan
- Advanced Materials, Vol. 21, Issue 17, p. 1665-1677
Atomic scale real-space mapping of holes in YBa2Cu3O6+δ
journal, July 2014
- Gauquelin, N.; Hawthorn, D. G.; Sawatzky, G. A.
- Nature Communications, Vol. 5, Issue 1
Raman and fluorescence contributions to the resonant inelastic soft x-ray scattering on heterostructures
journal, January 2018
- Pfaff, F.; Fujiwara, H.; Berner, G.
- Physical Review B, Vol. 97, Issue 3
Emergent phenomena at oxide interfaces
journal, January 2012
- Hwang, H. Y.; Iwasa, Y.; Kawasaki, M.
- Nature Materials, Vol. 11, Issue 2
Nanoscale control of an interfacial metal–insulator transition at room temperature
journal, March 2008
- Cen, C.; Thiel, S.; Hammerl, G.
- Nature Materials, Vol. 7, Issue 4
A high-mobility electron gas at the LaAlO3/SrTiO3 heterointerface
journal, January 2004
- Ohtomo, A.; Hwang, H. Y.
- Nature, Vol. 427, Issue 6973
Direct imaging of the electron liquid at oxide interfaces
journal, February 2018
- Song, Kyung; Ryu, Sangwoo; Lee, Hyungwoo
- Nature Nanotechnology, Vol. 13, Issue 3
Direct -Space Mapping of the Electronic Structure in an Oxide-Oxide Interface
journal, June 2013
- Berner, G.; Sing, M.; Fujiwara, H.
- Physical Review Letters, Vol. 110, Issue 24
Tunable Quasi-Two-Dimensional Electron Gases in Oxide Heterostructures
journal, September 2006
- Thiel, S.
- Science, Vol. 313, Issue 5795, p. 1942-1945
Why some interfaces cannot be sharp
journal, January 2006
- Nakagawa, Naoyuki; Hwang, Harold Y.; Muller, David A.
- Nature Materials, Vol. 5, Issue 3, p. 204-209
Momentum-resolved resonant inelastic soft X-ray scattering (qRIXS) endstation at the ALS
journal, October 2019
- Chuang, Yi-De; Feng, Xuefei; Cruz, Alejandro
- Journal of Electron Spectroscopy and Related Phenomena
A polarity-induced defect mechanism for conductivity and magnetism at polar–nonpolar oxide interfaces
journal, October 2014
- Yu, Liping; Zunger, Alex
- Nature Communications, Vol. 5, Issue 1
Polaronic metal state at the LaAlO3/SrTiO3 interface
journal, January 2016
- Cancellieri, C.; Mishchenko, A. S.; Aschauer, U.
- Nature Communications, Vol. 7, Issue 1
Structural and Electronic Reconstructions at the LaAlO 3 /SrTiO 3 Interface
journal, February 2013
- Salluzzo, M.; Gariglio, S.; Torrelles, X.
- Advanced Materials, Vol. 25, Issue 16
Polarity-induced oxygen vacancies at interfaces
journal, October 2010
- Zhong, Zhicheng; Xu, P. X.; Kelly, Paul J.
- Physical Review B, Vol. 82, Issue 16
Disentangling specific versus generic doping mechanisms in oxide heterointerfaces
journal, May 2017
- Gabel, J.; Zapf, M.; Scheiderer, P.
- Physical Review B, Vol. 95, Issue 19
Electronically coupled complementary interfaces between perovskite band insulators
journal, June 2006
- Huijben, Mark; Rijnders, Guus; Blank, Dave H. A.
- Nature Materials, Vol. 5, Issue 7
A polarity-induced defect mechanism for conductivity and magnetism at polar-nonpolar oxide interfaces
text, January 2014
- Yu, Liping; Zunger, Alex
- arXiv