Stoichiometry dependence of potential screening at interfaces
Abstract
Hard x-ray photoelectron spectroscopy (HAXPES) and variable kinetic energy x-ray photoelectron spectroscopy (VKE-XPS) analyses have been performed on ten-unit-cell-thick La(1-δ)Al(1+δ)O₃ films, with La:Al ratios of 1.1, 1.0, and 0.9, deposited on SrTiO₃. Only Al-rich films are known to have a conductive interface. VKE-XPS, coupled with maximum entropy analysis, shows significant differences in the compositional depth profile among the Al-rich, La-rich, and stoichiometric films: significant La enrichment at the interface is observed in the La-rich and stoichiometric films, while the Al-rich film shows little to no intermixing. Additionally, the La-rich and stoichiometric films show a high concentration of Al at the surface, which is not observed in the Al-rich film. HAXPES valence band (VB) analysis shows a broadening of the VB for the Al-rich sample relative to the stoichiometric and La-rich samples. This broadening is consistent with an electric field across the Al-rich film. These results are consistent with a defect-driven electronic reconstruction.
- Authors:
- Publication Date:
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1177475
- Grant/Contract Number:
- AC02-98CH10886
- Resource Type:
- Publisher's Accepted Manuscript
- Journal Name:
- Physical Review. B, Condensed Matter and Materials Physics
- Additional Journal Information:
- Journal Name: Physical Review. B, Condensed Matter and Materials Physics Journal Volume: 91 Journal Issue: 16; Journal ID: ISSN 1098-0121
- Publisher:
- American Physical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Weiland, Conan, Sterbinsky, George E., Rumaiz, Abdul K., Hellberg, C. Stephen, Woicik, Joseph C., Zhu, Shaobo, and Schlom, Darrell G. Stoichiometry dependence of potential screening at La ( 1 - δ ) Al ( 1 + δ ) O 3 / SrTiO 3 interfaces. United States: N. p., 2015.
Web. doi:10.1103/PhysRevB.91.165103.
Weiland, Conan, Sterbinsky, George E., Rumaiz, Abdul K., Hellberg, C. Stephen, Woicik, Joseph C., Zhu, Shaobo, & Schlom, Darrell G. Stoichiometry dependence of potential screening at La ( 1 - δ ) Al ( 1 + δ ) O 3 / SrTiO 3 interfaces. United States. https://doi.org/10.1103/PhysRevB.91.165103
Weiland, Conan, Sterbinsky, George E., Rumaiz, Abdul K., Hellberg, C. Stephen, Woicik, Joseph C., Zhu, Shaobo, and Schlom, Darrell G. Fri .
"Stoichiometry dependence of potential screening at La ( 1 - δ ) Al ( 1 + δ ) O 3 / SrTiO 3 interfaces". United States. https://doi.org/10.1103/PhysRevB.91.165103.
@article{osti_1177475,
title = {Stoichiometry dependence of potential screening at La ( 1 - δ ) Al ( 1 + δ ) O 3 / SrTiO 3 interfaces},
author = {Weiland, Conan and Sterbinsky, George E. and Rumaiz, Abdul K. and Hellberg, C. Stephen and Woicik, Joseph C. and Zhu, Shaobo and Schlom, Darrell G.},
abstractNote = {Hard x-ray photoelectron spectroscopy (HAXPES) and variable kinetic energy x-ray photoelectron spectroscopy (VKE-XPS) analyses have been performed on ten-unit-cell-thick La(1-δ)Al(1+δ)O₃ films, with La:Al ratios of 1.1, 1.0, and 0.9, deposited on SrTiO₃. Only Al-rich films are known to have a conductive interface. VKE-XPS, coupled with maximum entropy analysis, shows significant differences in the compositional depth profile among the Al-rich, La-rich, and stoichiometric films: significant La enrichment at the interface is observed in the La-rich and stoichiometric films, while the Al-rich film shows little to no intermixing. Additionally, the La-rich and stoichiometric films show a high concentration of Al at the surface, which is not observed in the Al-rich film. HAXPES valence band (VB) analysis shows a broadening of the VB for the Al-rich sample relative to the stoichiometric and La-rich samples. This broadening is consistent with an electric field across the Al-rich film. These results are consistent with a defect-driven electronic reconstruction.},
doi = {10.1103/PhysRevB.91.165103},
journal = {Physical Review. B, Condensed Matter and Materials Physics},
number = 16,
volume = 91,
place = {United States},
year = {Fri Apr 03 00:00:00 EDT 2015},
month = {Fri Apr 03 00:00:00 EDT 2015}
}
https://doi.org/10.1103/PhysRevB.91.165103
Web of Science
Works referenced in this record:
The electron attenuation length revisited
journal, June 2002
- Jablonski, A.
- Surface Science Reports, Vol. 47, Issue 2-3
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
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
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
Oxide Interfaces--An Opportunity for Electronics
journal, March 2010
- Mannhart, J.; Schlom, D. G.
- Science, Vol. 327, Issue 5973, p. 1607-1611
Nondestructive compositional depth profiling using variable-kinetic energy hard X-ray photoelectron spectroscopy and maximum entropy regularization: Depth profiling by VKE-XPS
journal, April 2014
- Weiland, C.; Krajewski, J.; Opila, R.
- Surface and Interface Analysis, Vol. 46, Issue 6
Hard x-ray photoemission and density functional theory study of the internal electric field in SrTiO /LaAlO oxide heterostructures
journal, February 2013
- Slooten, E.; Zhong, Zhicheng; Molegraaf, H. J. A.
- Physical Review B, Vol. 87, Issue 8
Understanding the mechanism of conductivity at the LaAlO3/SrTiO3(001) interface
journal, July 2011
- Chambers, Scott A.
- Surface Science, Vol. 605, Issue 13-14
PHOTOELECTRON ANGULAR DISTRIBUTION PARAMETERS FOR ELEMENTS Z=55 to Z=100 IN THE PHOTOELECTRON ENERGY RANGE 100–5000 eV
journal, November 2002
- Trzhaskovskaya, M. B.; Nefedov, V. I.; Yarzhemsky, V. G.
- Atomic Data and Nuclear Data Tables, Vol. 82, Issue 2
Hybridization and Bond-Orbital Components in Site-Specific X-Ray Photoelectron Spectra of Rutile
journal, July 2002
- Woicik, J. C.; Nelson, E. J.; Kronik, Leeor
- Physical Review Letters, Vol. 89, Issue 7
Polar-on-nonpolar epitaxy
journal, February 1987
- Kroemer, Herbert
- Journal of Crystal Growth, Vol. 81, Issue 1-4
Note: Alignment/focus dependent core-line sensitivity for quantitative chemical analysis in hard x-ray photoelectron spectroscopy using a hemispherical electron analyzer
journal, March 2013
- Weiland, Conan; Browning, Raymond; Karlin, Barry A.
- Review of Scientific Instruments, Vol. 84, Issue 3
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999
- Kresse, G.; Joubert, D.
- Physical Review B, Vol. 59, Issue 3, p. 1758-1775
LaAlO3 stoichiometry is key to electron liquid formation at LaAlO3/SrTiO3 interfaces
journal, August 2013
- Warusawithana, M. P.; Richter, C.; Mundy, J. A.
- Nature Communications, Vol. 4, Issue 1
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
Polar oxide surfaces
journal, July 2000
- Noguera, Claudine
- Journal of Physics: Condensed Matter, Vol. 12, Issue 31
PHOTOELECTRON ANGULAR DISTRIBUTION PARAMETERS FOR ELEMENTS Z=1 TO Z=54 IN THE PHOTOELECTRON ENERGY RANGE 100–5000 eV
journal, January 2001
- Trzhaskovskaya, M. B.; Nefedov, V. I.; Yarzhemsky, V. G.
- Atomic Data and Nuclear Data Tables, Vol. 77, Issue 1
Epitaxial SrTiO3 films with electron mobilities exceeding 30,000 cm2 V-1 s-1
journal, April 2010
- Son, Junwoo; Moetakef, Pouya; Jalan, Bharat
- Nature Materials, Vol. 9, Issue 6, p. 482-484
Band alignment in LaAlO /SrTiO oxide heterostructures inferred from hard x-ray photoelectron spectroscopy
journal, September 2013
- Berner, G.; Müller, A.; Pfaff, F.
- Physical Review B, Vol. 88, Issue 11
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
Origin of Charge Density at on Heterointerfaces: Possibility of Intrinsic Doping
journal, May 2007
- Siemons, Wolter; Koster, Gertjan; Yamamoto, Hideki
- Physical Review Letters, Vol. 98, Issue 19, Article No. 196802
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
Tunable Quasi-Two-Dimensional Electron Gases in Oxide Heterostructures
journal, September 2006
- Thiel, S.
- Science, Vol. 313, Issue 5795, p. 1942-1945
Oxygen vacancies in N doped anatase TiO2: Experiment and first-principles calculations
journal, December 2009
- Rumaiz, Abdul K.; Woicik, J. C.; Cockayne, E.
- Applied Physics Letters, Vol. 95, Issue 26
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
Built-in and induced polarization across LaAlO3/SrTiO3 heterojunctions
journal, October 2010
- Singh-Bhalla, Guneeta; Bell, Christopher; Ravichandran, Jayakanth
- Nature Physics, Vol. 7, Issue 1
Effect of Growth Induced (Non)Stoichiometry on Interfacial Conductance in
journal, May 2013
- Breckenfeld, E.; Bronn, N.; Karthik, J.
- Physical Review Letters, Vol. 110, Issue 19
The stability of ionic crystal surfaces
journal, November 1979
- Tasker, P. W.
- Journal of Physics C: Solid State Physics, Vol. 12, Issue 22
Effect of oxygen vacancies in the substrate on the electrical properties of the interface
journal, March 2007
- Kalabukhov, Alexey; Gunnarsson, Robert; Börjesson, Johan
- Physical Review B, Vol. 75, Issue 12
Instability, intermixing and electronic structure at the epitaxial LaAlO3/SrTiO3(001) heterojunction
journal, October 2010
- Chambers, S. A.; Engelhard, M. H.; Shutthanandan, V.
- Surface Science Reports, Vol. 65, Issue 10-12
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
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
Composition, structure, and stability of as a function of oxygen pressure
journal, December 2001
- Reuter, Karsten; Scheffler, Matthias
- Physical Review B, Vol. 65, Issue 3
X-ray photoemission studies of the metal-insulator transition in structures grown by molecular beam epitaxy
journal, December 2009
- Segal, Y.; Ngai, J. H.; Reiner, J. W.
- Physical Review B, Vol. 80, Issue 24
Simulation of electron spectra for surface analysis (SESSA): a novel software tool for quantitative Auger-electron spectroscopy and X-ray photoelectron spectroscopy
journal, January 2005
- Smekal, Werner; Werner, Wolfgang S. M.; Powell, Cedric J.
- Surface and Interface Analysis, Vol. 37, Issue 11