Atomic-scale structural and electronic properties of SrTiO3/GaAs interfaces: A combined STEM-EELS and first-principles study

Hong, Liang; Bhatnagar, Kunal; Droopad, Ravi; Klie, Robert F.; Öğüt, Serdar

doi:10.1103/PhysRevB.96.035311

Title: Atomic-scale structural and electronic properties of ${SrTiO}_{3} / GaAs$ interfaces: A combined STEM-EELS and first-principles study

Journal Article · Wed Jul 26 00:00:00 EDT 2017 · Physical Review B

DOI:https://doi.org/10.1103/PhysRevB.96.035311· OSTI ID:1544379

Hong, Liang ^[1]; Bhatnagar, Kunal ^[2]; Droopad, Ravi ^[2]; Klie, Robert F. ^[1]; Öğüt, Serdar ^[1]

Univ. of Illinois, Chicago, IL (United States). Dept. of Physics
Texas State Univ., San Marcos, TX (United States). Ingram School of Engineering

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.

View Accepted Manuscript (DOE)

View Accepted Manuscript (Publisher)

Cite

Export

Save

Research Organization:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Organization:: USDOE Office of Science (SC); National Science Foundation (NSF)

Grant/Contract Number:: AC02-05CH11231; DMR-1408427; DMR-0959470

OSTI ID:: 1544379

Alternate ID(s):: OSTI ID: 1372931

Journal Information:: Physical Review B, Vol. 96, Issue 3; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 4 works

Citation information provided by
Web of Science

References (48)

Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Interfacial and rectifying characteristic of epitaxial SrTiO3-δ/GaAs p–n junctions Wei, X. H.; Huang, W.; Yang, Z. B. Scripta Materialia, Vol. 65, Issue 4 https://doi.org/10.1016/j.scriptamat.2011.04.035	journal	August 2011
Atomic-scale imaging of nanoengineered oxygen vacancy profiles in SrTiO3 Muller, David A.; Nakagawa, Naoyuki; Ohtomo, Akira Nature, Vol. 430, Issue 7000 https://doi.org/10.1038/nature02756	journal	August 2004
Thermodynamic stability and growth kinetics of epitaxial SrTiO $_{3}$ on silicon Kolpak, A. M.; Ismail-Beigi, S. Physical Review B, Vol. 83, Issue 16 https://doi.org/10.1103/PhysRevB.83.165318	journal	April 2011
Atomic structure of epitaxial SrTiO3–GaAs(001) heterojunctions Klie, R. F.; Zhu, Y.; Altman, E. I. Applied Physics Letters, Vol. 87, Issue 14 https://doi.org/10.1063/1.2077837	journal	October 2005
Mechanism of cleaning Si(100) surface using Sr or SrO for the growth of crystalline SrTiO[sub 3] films Wei, Yi; Hu, Xiaoming; Liang, Yong Journal of Vacuum Science & Technology B: Microelectronics and Nanometer Structures, Vol. 20, Issue 4 https://doi.org/10.1116/1.1491547	journal	January 2002
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Electron counting model and its application to island structures on molecular-beam epitaxy grown GaAs(001) and ZnSe(001) Pashley, M. D. Physical Review B, Vol. 40, Issue 15 https://doi.org/10.1103/PhysRevB.40.10481	journal	November 1989
Band alignment at epitaxial SrTiO3–GaAs(001) heterojunction Liang, Y.; Curless, J.; McCready, D. Applied Physics Letters, Vol. 86, Issue 8 https://doi.org/10.1063/1.1871364	journal	February 2005
Band Offsets in Lattice-Matched Heterojunctions: A Model and First-Principles Calculations for GaAs/AlAs Baldereschi, Alfonso; Baroni, Stefano; Resta, Raffaele Physical Review Letters, Vol. 61, Issue 6 https://doi.org/10.1103/PhysRevLett.61.734	journal	August 1988
The effect of valence state and site geometry on Ti L3,2 and O K electron energy-loss spectra of TixOy phases Stoyanov, E.; Langenhorst, F.; Steinle-Neumann, G. American Mineralogist, Vol. 92, Issue 4 https://doi.org/10.2138/am.2007.2344	journal	April 2007
Watch out for the lack of oxygen Eckstein, James N. Nature Materials, Vol. 6, Issue 7 https://doi.org/10.1038/nmat1944	journal	July 2007
Atomic and electronic structures of SrTiO $_{3}$ /GaAs heterointerfaces: An 80-kV atomic-resolution electron energy-loss spectroscopy study Qiao, Q.; Klie, R. F.; Öğüt, S. Physical Review B, Vol. 85, Issue 16 https://doi.org/10.1103/PhysRevB.85.165406	journal	April 2012
Stable structure and effects of the substrate Ti pre-treatment on the epitaxial growth of SrTiO ₃ on GaAs Wang, Jianli; Wu, X. S.; Bai, Dongmei EPL (Europhysics Letters), Vol. 86, Issue 4 https://doi.org/10.1209/0295-5075/86/46008	journal	May 2009
Effect of oxygen vacancies in the ${SrTiO}_{3}$ substrate on the electrical properties of the ${LaAlO}_{3} ∕ {SrTiO}_{3}$ interface Kalabukhov, Alexey; Gunnarsson, Robert; Börjesson, Johan Physical Review B, Vol. 75, Issue 12 https://doi.org/10.1103/PhysRevB.75.121404	journal	March 2007
Surface Energy and the Common Dangling Bond Rule for Semiconductors Zhang, S. B.; Wei, Su-Huai Physical Review Letters, Vol. 92, Issue 8 https://doi.org/10.1103/PhysRevLett.92.086102	journal	February 2004
Composition, structure, and stability of ${RuO}_{2} (110)$ as a function of oxygen pressure Reuter, Karsten; Scheffler, Matthias Physical Review B, Vol. 65, Issue 3 https://doi.org/10.1103/PhysRevB.65.035406	journal	December 2001
Functional materials integrated on III–V semiconductors Gatabi, Javad; Lyon, Kevin; Rahman, Shafiqur Microelectronic Engineering, Vol. 147 https://doi.org/10.1016/j.mee.2015.04.050	journal	November 2015
Origin of the Two-Dimensional Electron Gas Carrier Density at the ${LaAlO}_{3}$ on ${SrTiO}_{3}$ Interface Popović, Zoran S.; Satpathy, Sashi; Martin, Richard M. Physical Review Letters, Vol. 101, Issue 25, Article No. 256801 https://doi.org/10.1103/PhysRevLett.101.256801	journal	December 2008
Two-dimensional electron gas with universal subbands at the surface of SrTiO₃ Santander-Syro, A. F.; Copie, O.; Kondo, T. Nature, Vol. 469, Issue 7329, p. 189-193 https://doi.org/10.1038/nature09720	journal	January 2011
${SrTiO}_{3} ∕ Si (001)$ epitaxial interface: A density functional theory study Yakovkin, I. N.; Gutowski, M. Physical Review B, Vol. 70, Issue 16 https://doi.org/10.1103/PhysRevB.70.165319	journal	October 2004
The new JEOL JEM-ARM200CF at the University of Illinois at Chicago: The new JEOL JEM-ARM200CF at the University of Illinois at Chicago Klie, R. F.; Gulec, A.; Guo, Z. Crystal Research and Technology, Vol. 49, Issue 9 https://doi.org/10.1002/crat.201300200	journal	September 2013
Magnetic effects at the interface between non-magnetic oxides Brinkman, A.; Huijben, M.; van Zalk, M. Nature Materials, Vol. 6, Issue 7, p. 493-496 https://doi.org/10.1038/nmat1931	journal	June 2007
Crystalline Oxides on Silicon: The First Five Monolayers McKee, R. A.; Walker, F. J.; Chisholm, M. F. Physical Review Letters, Vol. 81, Issue 14 https://doi.org/10.1103/PhysRevLett.81.3014	journal	October 1998
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Kresse, G.; Furthmüller, J. Computational Materials Science, Vol. 6, Issue 1, p. 15-50 https://doi.org/10.1016/0927-0256(96)00008-0	journal	July 1996
Direct observation of oxygen-vacancy-enhanced polarization in a SrTiO3-buffered ferroelectric BaTiO3 film on GaAs Qiao, Qiao; Zhang, Yuyang; Contreras-Guerrero, Rocio Applied Physics Letters, Vol. 107, Issue 20 https://doi.org/10.1063/1.4936159	journal	November 2015
Molecular beam epitaxy of SrTiO3 on GaAs(001): GaAs surface treatment and structural characterization of the oxide layer Louahadj, L.; Bachelet, R.; Regreny, P. Thin Solid Films, Vol. 563 https://doi.org/10.1016/j.tsf.2014.02.062	journal	July 2014
GaAs MESFETs fabricated on Si substrates using a SrTiO ₃ buffer layer Eisenbeiser, K.; Emrick, R.; Droopad, R. IEEE Electron Device Letters, Vol. 23, Issue 6 https://doi.org/10.1109/LED.2002.1004215	journal	June 2002
Structural and dielectric properties of epitaxial SrTiO3 films grown directly on GaAs substrates by laser molecular beam epitaxy Wu, Z. P.; Huang, W.; Wong, K. H. Journal of Applied Physics, Vol. 104, Issue 5 https://doi.org/10.1063/1.2974796	journal	September 2008
Interface structure and film polarization in epitaxial SrTiO $_{3}$ /Si(001) Kolpak, A. M.; Ismail-Beigi, S. Physical Review B, Vol. 85, Issue 19 https://doi.org/10.1103/PhysRevB.85.195318	journal	May 2012
First-principles study of the atomic reconstructions and energies of Ga- and As-stabilized GaAs(100) surfaces Qian, Guo-Xin; Martin, Richard M.; Chadi, D. J. Physical Review B, Vol. 38, Issue 11 https://doi.org/10.1103/PhysRevB.38.7649	journal	October 1988
Structure of ${SrTiO}_{3}$ Films on Si Hellberg, C. Stephen; Andersen, Kristopher E.; Li, Hao Physical Review Letters, Vol. 108, Issue 16 https://doi.org/10.1103/PhysRevLett.108.166101	journal	April 2012
Density-Functional Theory of Excitation Spectra of Semiconductors: Application to Si Wang, C. S.; Pickett, W. E. Physical Review Letters, Vol. 51, Issue 7 https://doi.org/10.1103/PhysRevLett.51.597	journal	August 1983
A high-mobility electron gas at the LaAlO3/SrTiO3 heterointerface Ohtomo, A.; Hwang, H. Y. Nature, Vol. 427, Issue 6973 https://doi.org/10.1038/nature02308	journal	January 2004
Origin of Charge Density at ${LaAlO}_{3}$ on ${SrTiO}_{3}$ Heterointerfaces: Possibility of Intrinsic Doping Siemons, Wolter; Koster, Gertjan; Yamamoto, Hideki Physical Review Letters, Vol. 98, Issue 19, Article No. 196802 https://doi.org/10.1103/PhysRevLett.98.196802	journal	May 2007
Crystallographic relationships between GaAs, As and Ga2O3 at the GaAs-thermal oxide interface Sands, T.; Washburn, J.; Gronsky, R. Materials Letters, Vol. 3, Issue 5-6 https://doi.org/10.1016/0167-577X(85)90066-7	journal	April 1985
Perspectives on III–V compound MIS structures Wieder, H. H. Journal of Vacuum Science and Technology, Vol. 15, Issue 4 https://doi.org/10.1116/1.569773	journal	July 1978
Why some interfaces cannot be sharp Nakagawa, Naoyuki; Hwang, Harold Y.; Muller, David A. Nature Materials, Vol. 5, Issue 3, p. 204-209 https://doi.org/10.1038/nmat1569	journal	January 2006
Tunable Quasi-Two-Dimensional Electron Gases in Oxide Heterostructures Thiel, S. Science, Vol. 313, Issue 5795, p. 1942-1945 https://doi.org/10.1126/science.1131091	journal	September 2006
Properties of epitaxial BaTiO ₃ deposited on GaAs Contreras-Guerrero, R.; Veazey, J. P.; Levy, J. Applied Physics Letters, Vol. 102, Issue 1 https://doi.org/10.1063/1.4773988	journal	January 2013
The role of titanium at the SrTiO 3 /GaAs epitaxial interface Meunier, B.; Bachelet, R.; Grenet, G. Journal of Crystal Growth, Vol. 433 https://doi.org/10.1016/j.jcrysgro.2015.10.013	journal	January 2016
$Sr Ti O_{3}$ substrates capped with a GaAs monolayer: An ab initio study Bottin, François; Finocchi, Fabio Physical Review B, Vol. 76, Issue 16 https://doi.org/10.1103/PhysRevB.76.165427	journal	October 2007
2p X-ray absorption of titanium in minerals de Groot, F. M. F.; Figueiredo, M. O.; Basto, M. J. Physics and Chemistry of Minerals, Vol. 19, Issue 3 https://doi.org/10.1007/BF00202101	journal	September 1992
The influence of atomic structure on the formation of electrical barriers at grain boundaries in SrTiO3 Browning, N. D.; Buban, J. P.; Moltaji, H. O. Applied Physics Letters, Vol. 74, Issue 18 https://doi.org/10.1063/1.123922	journal	May 1999
Recent studies of oxide-semiconductor heterostructures using aberration-corrected scanning transmission electron microscopy Smith, David J.; Wu, HsinWei; Lu, Sirong Journal of Materials Research, Vol. 32, Issue 5 https://doi.org/10.1557/jmr.2016.273	journal	August 2016
Development of integrated heterostructures on silicon by MBE Droopad, Ravi; Yu, Zhiyi; Li, Hao Journal of Crystal Growth, Vol. 251, Issue 1-4 https://doi.org/10.1016/S0022-0248(02)02200-5	journal	April 2003
Transmission Electron Microscopic and First-principles Study of SrTiO3/GaAs Hetero-interfaces Hong, Liang; Ögüt, Serdar; Klie, Robert Microscopy and Microanalysis, Vol. 21, Issue S3 https://doi.org/10.1017/S1431927615009010	journal	August 2015
Hetero-epitaxy of perovskite oxides on GaAs(001) by molecular beam epitaxy Liang, Y.; Kulik, J.; Eschrich, T. C. Applied Physics Letters, Vol. 85, Issue 7 https://doi.org/10.1063/1.1783016	journal	August 2004

Cited By (1)

Epitaxial Oxides on Semiconductors: From Fundamentals to New Devices Kumah, Divine P.; Ngai, Joseph H.; Kornblum, Lior Advanced Functional Materials https://doi.org/10.1002/adfm.201901597	journal	July 2019

Similar Records

Dynamic interface rearrangement in

{LaFeO}_{3} / n - {SrTiO}_{3}

heterojunctions

Journal Article · Mon Nov 06 00:00:00 EST 2017 · Physical Review Materials · OSTI ID:1544379

Spurgeon, Steven R.; Sushko, Peter V.; Chambers, Scott A.; +1 more

Surface and interface properties of

L a_{2 / 3} S r_{1 / 3} Mn O_{3}

thin films on

{SrTiO}_{3}

(001)

Journal Article · Mon Apr 22 00:00:00 EDT 2019 · Physical Review Materials · OSTI ID:1544379

Chen, Lina; Wang, Zhen; Wang, Gaomin; +6 more

Observation of Out-of-Plane Spin Texture in a

{SrTiO}_{3} (111)

Two-Dimensional Electron Gas

Journal Article · Fri Jun 29 00:00:00 EDT 2018 · Physical Review Letters · OSTI ID:1544379

He, Pan; Walker, S. McKeown; Zhang, Steven S. -L.; +9 more

Related Subjects

75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY

Title: Atomic-scale structural and electronic properties of SrTiO 3 / GaAs interfaces: A combined STEM-EELS and first-principles study

Citation Formats

References (48)

Cited By (1)

Similar Records

Related Subjects

Title: Atomic-scale structural and electronic properties of ${SrTiO}_{3} / GaAs$ interfaces: A combined STEM-EELS and first-principles study