Atomic-scale structural and electronic properties of interfaces: A combined STEM-EELS and first-principles study
Abstract
The electronic properties of epitaxial oxide thin films grown on compound semiconductors are largely determined by the interfacial atomic structure, as well as the thermodynamic conditions during synthesis. Ferroelectric polarization and Fermi-level pinning in SrTiO3 films have been attributed to the presence of oxygen vacancies at the oxide/semiconductor interface. Here, we present scanning transmission electron microscopy (STEM) and electron energy-loss spectroscopy analyses of GaAs films grown on SrTiO3 combined with first-principles calculations to determine the atomic and electronic structures of the SrTiO3/GaAs interfaces. In this work, an atomically abrupt SrO/As interface is observed and the interfacial SrO layer is found to be O-deficient. First-principles density functional theory (DFT) calculations show SrO/Ga and Sr/As interfaces are favorable under O-rich and O-poor conditions, respectively. The SrO/Ga interface is reconstructed via the formation of Ga-Ga dimers while the Sr/As interface is abrupt and consistent with the experiment. DFT calculations further reveal that intrinsic two-dimensional electron gas (2DEG) forms in both SrO/Ga and Sr/As interfaces, and the Fermi level is pinned to the localized 2DEG states. Interfacial O vacancies can enhance the 2DEG density while it is possible for Ga/As vacancies to unpin the Fermi level from the 2DEG states.
- Authors:
-
- Univ. of Illinois, Chicago, IL (United States). Dept. of Physics
- Texas State Univ., San Marcos, TX (United States). Ingram School of Engineering
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
- Sponsoring Org.:
- USDOE Office of Science (SC); National Science Foundation (NSF)
- OSTI Identifier:
- 1544379
- Alternate Identifier(s):
- OSTI ID: 1372931
- Grant/Contract Number:
- AC02-05CH11231; DMR-1408427; DMR-0959470
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review B
- Additional Journal Information:
- Journal Volume: 96; Journal Issue: 3; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY
Citation Formats
Hong, Liang, Bhatnagar, Kunal, Droopad, Ravi, Klie, Robert F., and Öğüt, Serdar. Atomic-scale structural and electronic properties of SrTiO3/GaAs interfaces: A combined STEM-EELS and first-principles study. United States: N. p., 2017.
Web. doi:10.1103/PhysRevB.96.035311.
Hong, Liang, Bhatnagar, Kunal, Droopad, Ravi, Klie, Robert F., & Öğüt, Serdar. Atomic-scale structural and electronic properties of SrTiO3/GaAs interfaces: A combined STEM-EELS and first-principles study. United States. https://doi.org/10.1103/PhysRevB.96.035311
Hong, Liang, Bhatnagar, Kunal, Droopad, Ravi, Klie, Robert F., and Öğüt, Serdar. Wed .
"Atomic-scale structural and electronic properties of SrTiO3/GaAs interfaces: A combined STEM-EELS and first-principles study". United States. https://doi.org/10.1103/PhysRevB.96.035311. https://www.osti.gov/servlets/purl/1544379.
@article{osti_1544379,
title = {Atomic-scale structural and electronic properties of SrTiO3/GaAs interfaces: A combined STEM-EELS and first-principles study},
author = {Hong, Liang and Bhatnagar, Kunal and Droopad, Ravi and Klie, Robert F. and Öğüt, Serdar},
abstractNote = {The electronic properties of epitaxial oxide thin films grown on compound semiconductors are largely determined by the interfacial atomic structure, as well as the thermodynamic conditions during synthesis. Ferroelectric polarization and Fermi-level pinning in SrTiO3 films have been attributed to the presence of oxygen vacancies at the oxide/semiconductor interface. Here, we present scanning transmission electron microscopy (STEM) and electron energy-loss spectroscopy analyses of GaAs films grown on SrTiO3 combined with first-principles calculations to determine the atomic and electronic structures of the SrTiO3/GaAs interfaces. In this work, an atomically abrupt SrO/As interface is observed and the interfacial SrO layer is found to be O-deficient. First-principles density functional theory (DFT) calculations show SrO/Ga and Sr/As interfaces are favorable under O-rich and O-poor conditions, respectively. The SrO/Ga interface is reconstructed via the formation of Ga-Ga dimers while the Sr/As interface is abrupt and consistent with the experiment. DFT calculations further reveal that intrinsic two-dimensional electron gas (2DEG) forms in both SrO/Ga and Sr/As interfaces, and the Fermi level is pinned to the localized 2DEG states. Interfacial O vacancies can enhance the 2DEG density while it is possible for Ga/As vacancies to unpin the Fermi level from the 2DEG states.},
doi = {10.1103/PhysRevB.96.035311},
journal = {Physical Review B},
number = 3,
volume = 96,
place = {United States},
year = {Wed Jul 26 00:00:00 EDT 2017},
month = {Wed Jul 26 00:00:00 EDT 2017}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 4 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
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
Interfacial and rectifying characteristic of epitaxial SrTiO3-δ/GaAs p–n junctions
journal, August 2011
- Wei, X. H.; Huang, W.; Yang, Z. B.
- Scripta Materialia, Vol. 65, Issue 4
Atomic-scale imaging of nanoengineered oxygen vacancy profiles in SrTiO3
journal, August 2004
- Muller, David A.; Nakagawa, Naoyuki; Ohtomo, Akira
- Nature, Vol. 430, Issue 7000
Thermodynamic stability and growth kinetics of epitaxial SrTiO on silicon
journal, April 2011
- Kolpak, A. M.; Ismail-Beigi, S.
- Physical Review B, Vol. 83, Issue 16
Atomic structure of epitaxial SrTiO3–GaAs(001) heterojunctions
journal, October 2005
- Klie, R. F.; Zhu, Y.; Altman, E. I.
- Applied Physics Letters, Vol. 87, Issue 14
Mechanism of cleaning Si(100) surface using Sr or SrO for the growth of crystalline SrTiO[sub 3] films
journal, January 2002
- Wei, Yi; Hu, Xiaoming; Liang, Yong
- Journal of Vacuum Science & Technology B: Microelectronics and Nanometer Structures, Vol. 20, Issue 4
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
Electron counting model and its application to island structures on molecular-beam epitaxy grown GaAs(001) and ZnSe(001)
journal, November 1989
- Pashley, M. D.
- Physical Review B, Vol. 40, Issue 15
Band alignment at epitaxial SrTiO3–GaAs(001) heterojunction
journal, February 2005
- Liang, Y.; Curless, J.; McCready, D.
- Applied Physics Letters, Vol. 86, Issue 8
Band Offsets in Lattice-Matched Heterojunctions: A Model and First-Principles Calculations for GaAs/AlAs
journal, August 1988
- Baldereschi, Alfonso; Baroni, Stefano; Resta, Raffaele
- Physical Review Letters, Vol. 61, Issue 6
The effect of valence state and site geometry on Ti L3,2 and O K electron energy-loss spectra of TixOy phases
journal, April 2007
- Stoyanov, E.; Langenhorst, F.; Steinle-Neumann, G.
- American Mineralogist, Vol. 92, Issue 4
Watch out for the lack of oxygen
journal, July 2007
- Eckstein, James N.
- Nature Materials, Vol. 6, Issue 7
Atomic and electronic structures of SrTiO /GaAs heterointerfaces: An 80-kV atomic-resolution electron energy-loss spectroscopy study
journal, April 2012
- Qiao, Q.; Klie, R. F.; Öğüt, S.
- Physical Review B, Vol. 85, Issue 16
Stable structure and effects of the substrate Ti pre-treatment on the epitaxial growth of SrTiO 3 on GaAs
journal, May 2009
- Wang, Jianli; Wu, X. S.; Bai, Dongmei
- EPL (Europhysics Letters), Vol. 86, Issue 4
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
Surface Energy and the Common Dangling Bond Rule for Semiconductors
journal, February 2004
- Zhang, S. B.; Wei, Su-Huai
- Physical Review Letters, Vol. 92, Issue 8
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
Functional materials integrated on III–V semiconductors
journal, November 2015
- Gatabi, Javad; Lyon, Kevin; Rahman, Shafiqur
- Microelectronic Engineering, Vol. 147
Origin of the Two-Dimensional Electron Gas Carrier Density at the on Interface
journal, December 2008
- Popović, Zoran S.; Satpathy, Sashi; Martin, Richard M.
- Physical Review Letters, Vol. 101, Issue 25, Article No. 256801
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
epitaxial interface: A density functional theory study
journal, October 2004
- Yakovkin, I. N.; Gutowski, M.
- Physical Review B, Vol. 70, Issue 16
The new JEOL JEM-ARM200CF at the University of Illinois at Chicago: The new JEOL JEM-ARM200CF at the University of Illinois at Chicago
journal, September 2013
- Klie, R. F.; Gulec, A.; Guo, Z.
- Crystal Research and Technology, Vol. 49, Issue 9
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
Crystalline Oxides on Silicon: The First Five Monolayers
journal, October 1998
- McKee, R. A.; Walker, F. J.; Chisholm, M. F.
- Physical Review Letters, Vol. 81, Issue 14
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996
- Kresse, G.; Furthmüller, J.
- Computational Materials Science, Vol. 6, Issue 1, p. 15-50
Direct observation of oxygen-vacancy-enhanced polarization in a SrTiO3-buffered ferroelectric BaTiO3 film on GaAs
journal, November 2015
- Qiao, Qiao; Zhang, Yuyang; Contreras-Guerrero, Rocio
- Applied Physics Letters, Vol. 107, Issue 20
Molecular beam epitaxy of SrTiO3 on GaAs(001): GaAs surface treatment and structural characterization of the oxide layer
journal, July 2014
- Louahadj, L.; Bachelet, R.; Regreny, P.
- Thin Solid Films, Vol. 563
GaAs MESFETs fabricated on Si substrates using a SrTiO 3 buffer layer
journal, June 2002
- Eisenbeiser, K.; Emrick, R.; Droopad, R.
- IEEE Electron Device Letters, Vol. 23, Issue 6
Structural and dielectric properties of epitaxial SrTiO3 films grown directly on GaAs substrates by laser molecular beam epitaxy
journal, September 2008
- Wu, Z. P.; Huang, W.; Wong, K. H.
- Journal of Applied Physics, Vol. 104, Issue 5
Interface structure and film polarization in epitaxial SrTiO /Si(001)
journal, May 2012
- Kolpak, A. M.; Ismail-Beigi, S.
- Physical Review B, Vol. 85, Issue 19
First-principles study of the atomic reconstructions and energies of Ga- and As-stabilized GaAs(100) surfaces
journal, October 1988
- Qian, Guo-Xin; Martin, Richard M.; Chadi, D. J.
- Physical Review B, Vol. 38, Issue 11
Structure of Films on Si
journal, April 2012
- Hellberg, C. Stephen; Andersen, Kristopher E.; Li, Hao
- Physical Review Letters, Vol. 108, Issue 16
Density-Functional Theory of Excitation Spectra of Semiconductors: Application to Si
journal, August 1983
- Wang, C. S.; Pickett, W. E.
- Physical Review Letters, Vol. 51, Issue 7
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
Crystallographic relationships between GaAs, As and Ga2O3 at the GaAs-thermal oxide interface
journal, April 1985
- Sands, T.; Washburn, J.; Gronsky, R.
- Materials Letters, Vol. 3, Issue 5-6
Perspectives on III–V compound MIS structures
journal, July 1978
- Wieder, H. H.
- Journal of Vacuum Science and Technology, Vol. 15, Issue 4
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
Properties of epitaxial BaTiO 3 deposited on GaAs
journal, January 2013
- Contreras-Guerrero, R.; Veazey, J. P.; Levy, J.
- Applied Physics Letters, Vol. 102, Issue 1
The role of titanium at the SrTiO 3 /GaAs epitaxial interface
journal, January 2016
- Meunier, B.; Bachelet, R.; Grenet, G.
- Journal of Crystal Growth, Vol. 433
substrates capped with a GaAs monolayer: An ab initio study
journal, October 2007
- Bottin, François; Finocchi, Fabio
- Physical Review B, Vol. 76, Issue 16
2p X-ray absorption of titanium in minerals
journal, September 1992
- de Groot, F. M. F.; Figueiredo, M. O.; Basto, M. J.
- Physics and Chemistry of Minerals, Vol. 19, Issue 3
The influence of atomic structure on the formation of electrical barriers at grain boundaries in SrTiO3
journal, May 1999
- Browning, N. D.; Buban, J. P.; Moltaji, H. O.
- Applied Physics Letters, Vol. 74, Issue 18
Recent studies of oxide-semiconductor heterostructures using aberration-corrected scanning transmission electron microscopy
journal, August 2016
- Smith, David J.; Wu, HsinWei; Lu, Sirong
- Journal of Materials Research, Vol. 32, Issue 5
Development of integrated heterostructures on silicon by MBE
journal, April 2003
- Droopad, Ravi; Yu, Zhiyi; Li, Hao
- Journal of Crystal Growth, Vol. 251, Issue 1-4
Transmission Electron Microscopic and First-principles Study of SrTiO3/GaAs Hetero-interfaces
journal, August 2015
- Hong, Liang; Ögüt, Serdar; Klie, Robert
- Microscopy and Microanalysis, Vol. 21, Issue S3
Hetero-epitaxy of perovskite oxides on GaAs(001) by molecular beam epitaxy
journal, August 2004
- Liang, Y.; Kulik, J.; Eschrich, T. C.
- Applied Physics Letters, Vol. 85, Issue 7
Works referencing / citing this record:
Epitaxial Oxides on Semiconductors: From Fundamentals to New Devices
journal, July 2019
- Kumah, Divine P.; Ngai, Joseph H.; Kornblum, Lior
- Advanced Functional Materials