Direct observation of a two-dimensional hole gas at oxide interfaces
Abstract
The discovery of a two-dimensional electron gas (2DEG) at the LaAlO3/SrTiO3 interface has resulted in the observation of many properties not present in conventional semiconductor heterostructures, and so become a focal point for device applications. Its counterpart, the two-dimensional hole gas (2DHG), is expected to complement the 2DEG. However, although the 2DEG has been widely observed, the 2DHG has proved elusive. Here in this paper we demonstrate a highly mobile 2DHG in epitaxially grown SrTiO3/LaAlO3/SrTiO3 heterostructures. Using electrical transport measurements and in-line electron holography, we provide direct evidence of a 2DHG that coexists with a 2DEG at complementary heterointerfaces in the same structure. First-principles calculations, coherent Bragg rod analysis and depth-resolved cathodoluminescence spectroscopy consistently support our finding that to eliminate ionic point defects is key to realizing a 2DHG. Lastly, the coexistence of a 2DEG and a 2DHG in a single oxide heterostructure provides a platform for the exciting physics of confined electron-hole systems and for developing applications.
- Authors:
-
[7];
- Univ. of Wisconsin, Madison, WI (United States). Dept. of Materials Science and Engineering
- Univ. of Wisconsin, Madison, WI (United States). Dept. of Physics
- Sungkyunkwan Univ., Suwon (Republic of Korea). Dept. of Energy Science
- The Ohio State Univ., Columbus, OH (United States). Dept. of Physics
- Univ. of Nebraska, Lincoln, NE (United States). Nebraska Center for Materials and Nanoscience, Dept. of Physics and Astronomy
- Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS), X-Ray Science Division
- Sungkyunkwan Univ., Suwon (Republic of Korea). Dept. of Energy Science; Pohang Univ. of Science and Technology (POSTECH) (Korea, Republic of). Dept. of Materials Science and Engineering
- The Ohio State Univ., Columbus, OH (United States). Dept. of Physics; The Ohio State Univ., Columbus, OH (United States). Dept. of Electrical and Computer Engineering
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1469800
- Grant/Contract Number:
- AC02-06CH11357; FG02-06ER46327; DMR-1629270; DMR-1420645; DMR-1305193; FA9550-15-1-0334; FA2386-15-1-4046
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Materials
- Additional Journal Information:
- Journal Volume: 17; Journal Issue: 3; Journal ID: ISSN 1476-1122
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Lee, H., Campbell, N., Lee, J., Asel, T. J., Paudel, T. R., Zhou, H., Lee, J. W., Noesges, B., Seo, J., Park, B., Brillson, L. J., Oh, S. H., Tsymbal, E. Y., Rzchowski, M. S., and Eom, C. B. Direct observation of a two-dimensional hole gas at oxide interfaces. United States: N. p., 2018.
Web. doi:10.1038/s41563-017-0002-4.
Lee, H., Campbell, N., Lee, J., Asel, T. J., Paudel, T. R., Zhou, H., Lee, J. W., Noesges, B., Seo, J., Park, B., Brillson, L. J., Oh, S. H., Tsymbal, E. Y., Rzchowski, M. S., & Eom, C. B. Direct observation of a two-dimensional hole gas at oxide interfaces. United States. doi:10.1038/s41563-017-0002-4.
Lee, H., Campbell, N., Lee, J., Asel, T. J., Paudel, T. R., Zhou, H., Lee, J. W., Noesges, B., Seo, J., Park, B., Brillson, L. J., Oh, S. H., Tsymbal, E. Y., Rzchowski, M. S., and Eom, C. B. Mon .
"Direct observation of a two-dimensional hole gas at oxide interfaces". United States. doi:10.1038/s41563-017-0002-4. https://www.osti.gov/servlets/purl/1469800.
@article{osti_1469800,
title = {Direct observation of a two-dimensional hole gas at oxide interfaces},
author = {Lee, H. and Campbell, N. and Lee, J. and Asel, T. J. and Paudel, T. R. and Zhou, H. and Lee, J. W. and Noesges, B. and Seo, J. and Park, B. and Brillson, L. J. and Oh, S. H. and Tsymbal, E. Y. and Rzchowski, M. S. and Eom, C. B.},
abstractNote = {The discovery of a two-dimensional electron gas (2DEG) at the LaAlO3/SrTiO3 interface has resulted in the observation of many properties not present in conventional semiconductor heterostructures, and so become a focal point for device applications. Its counterpart, the two-dimensional hole gas (2DHG), is expected to complement the 2DEG. However, although the 2DEG has been widely observed, the 2DHG has proved elusive. Here in this paper we demonstrate a highly mobile 2DHG in epitaxially grown SrTiO3/LaAlO3/SrTiO3 heterostructures. Using electrical transport measurements and in-line electron holography, we provide direct evidence of a 2DHG that coexists with a 2DEG at complementary heterointerfaces in the same structure. First-principles calculations, coherent Bragg rod analysis and depth-resolved cathodoluminescence spectroscopy consistently support our finding that to eliminate ionic point defects is key to realizing a 2DHG. Lastly, the coexistence of a 2DEG and a 2DHG in a single oxide heterostructure provides a platform for the exciting physics of confined electron-hole systems and for developing applications.},
doi = {10.1038/s41563-017-0002-4},
journal = {Nature Materials},
number = 3,
volume = 17,
place = {United States},
year = {2018},
month = {2}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 27 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:
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
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
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
Extreme mobility enhancement of two-dimensional electron gases at oxide interfaces by charge-transfer-induced modulation doping
journal, June 2015
- Chen, Y. Z.; Trier, F.; Wijnands, T.
- Nature Materials, Vol. 14, Issue 8
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
Highly efficient and tunable spin-to-charge conversion through Rashba coupling at oxide interfaces
journal, August 2016
- Lesne, E.; Fu, Yu; Oyarzun, S.
- Nature Materials, Vol. 15, Issue 12
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
Sketched oxide single-electron transistor
journal, April 2011
- Cheng, Guanglei; Siles, Pablo F.; Bi, Feng
- Nature Nanotechnology, Vol. 6, Issue 6
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
Strain on ferroelectric thin films: Example of Pb(Zr1−xTix)O3
journal, October 2009
- Janolin, Pierre-Eymeric
- Journal of Materials Science, Vol. 44, Issue 19
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
Two-Dimensional Electron Gases at Oxide Interfaces
journal, November 2008
- Mannhart, J.; Blank, D. H. A.; Hwang, H. Y.
- MRS Bulletin, Vol. 33, Issue 11
Charge localization or itineracy at interfaces Hole polarons, oxygen vacancies, and mobile electrons
journal, July 2006
- Pentcheva, R.; Pickett, W. E.
- Physical Review B, Vol. 74, Issue 3, Article No. 035112
Electric field control of the LaAlO3/SrTiO3 interface ground state
journal, December 2008
- Caviglia, A. D.; Gariglio, S.; Reyren, N.
- Nature, Vol. 456, Issue 7222
A flux-preserving non-linear inline holography reconstruction algorithm for partially coherent electrons
journal, January 2008
- Koch, Christoph T.
- Ultramicroscopy, Vol. 108, Issue 2
Towards full-resolution inline electron holography
journal, August 2014
- Koch, Christoph T.
- Micron, Vol. 63
Tailoring a two-dimensional electron gas at the LaAlO3/SrTiO3 (001) interface by epitaxial strain
journal, February 2011
- Bark, C. W.; Felker, D. A.; Wang, Y.
- Proceedings of the National Academy of Sciences, Vol. 108, Issue 12
Emergent phenomena at oxide interfaces
journal, January 2012
- Hwang, H. Y.; Iwasa, Y.; Kawasaki, M.
- Nature Materials, Vol. 11, Issue 2
A high-mobility electron gas at the LaAlO3/SrTiO3 heterointerface
journal, January 2004
- Ohtomo, A.; Hwang, H. Y.
- Nature, Vol. 427, Issue 6973
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
Excitonic binding in coupled quantum wells
journal, May 2003
- Szymanska, M. H.; Littlewood, P. B.
- Physical Review B, Vol. 67, Issue 19
Superconducting Interfaces Between Insulating Oxides
journal, August 2007
- Reyren, N.; Thiel, S.; Caviglia, A. D.
- Science, Vol. 317, Issue 5842
Anomalous expansion of the copper-apical-oxygen distance in superconducting cuprate bilayers
journal, April 2010
- Zhou, H.; Yacoby, Y.; Butko, V. Y.
- Proceedings of the National Academy of Sciences, Vol. 107, Issue 18
Bose–Einstein condensation of excitons in bilayer electron systems
journal, December 2004
- Eisenstein, J. P.; MacDonald, A. H.
- Nature, Vol. 432, Issue 7018
Polarity-induced oxygen vacancies at interfaces
journal, October 2010
- Zhong, Zhicheng; Xu, P. X.; Kelly, Paul J.
- Physical Review B, Vol. 82, Issue 16
Applications of depth-resolved cathodoluminescence spectroscopy
journal, April 2012
- Brillson, L. J.
- Journal of Physics D: Applied Physics, Vol. 45, Issue 18
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
Optical identification of oxygen vacancy formation at SrTiO 3 –(Ba,Sr)TiO 3 heterostructures
journal, May 2014
- Rutkowski, M. M.; McNicholas, K.; Zeng, Z. Q.
- Journal of Physics D: Applied Physics, Vol. 47, Issue 25
Local probing of coupled interfaces between two-dimensional electron and hole gases in oxide heterostructures by variable-temperature scanning tunneling spectroscopy
journal, July 2012
- Huijben, M.; Kockmann, D.; Huijben, J.
- Physical Review B, Vol. 86, Issue 3
Tunable Rashba Spin-Orbit Interaction at Oxide Interfaces
journal, March 2010
- Caviglia, A. D.; Gabay, M.; Gariglio, S.
- Physical Review Letters, Vol. 104, Issue 12, Article No. 126803
Electron-hole liquids in transition-metal oxide heterostructures
journal, August 2010
- Millis, A. J.; Schlom, Darrell G.
- Physical Review B, Vol. 82, Issue 7
The limits of ultrahigh-resolution x-ray mapping: estimating uncertainties in thin-film and interface structures determined by phase retrieval methods
journal, April 2012
- Zhou, Hua; Pindak, Ron; Clarke, Roy
- Journal of Physics D: Applied Physics, Vol. 45, Issue 19
Influence of atomic termination on the LaAlO /SrTiO interfacial polar rearrangement
journal, July 2013
- Rubano, A.; Günter, T.; Fink, T.
- Physical Review B, Vol. 88, Issue 3
Depth-resolved subsurface defects in chemically etched SrTiO3
journal, March 2009
- Zhang, Jun; Doutt, D.; Merz, T.
- Applied Physics Letters, Vol. 94, Issue 9
Charge compensation and mixed valency in heterointerfaces studied by the FLAPW method
journal, November 2006
- Park, Min Sik; Rhim, S. H.; Freeman, Arthur J.
- Physical Review B, Vol. 74, Issue 20
First-principles study of the mobility of
journal, December 2014
- Himmetoglu, Burak; Janotti, Anderson; Peelaers, Hartwin
- Physical Review B, Vol. 90, Issue 24
Structural and electronic properties of -doped and -doped
journal, December 2004
- Luo, Weidong; Duan, Wenhui; Louie, Steven G.
- Physical Review B, Vol. 70, Issue 21
Coulomb drag and spin drag in the presence of spin-orbit coupling
journal, January 2007
- Tse, Wang-Kong; Das Sarma, S.
- Physical Review B, Vol. 75, Issue 4
Polaronic metal state at the LaAlO3/SrTiO3 interface
journal, January 2016
- Cancellieri, C.; Mishchenko, A. S.; Aschauer, U.
- Nature Communications, Vol. 7, Issue 1
Room-temperature electronically-controlled ferromagnetism at the LaAlO3/SrTiO3 interface
journal, September 2014
- Bi, Feng; Huang, Mengchen; Ryu, Sangwoo
- Nature Communications, Vol. 5, Issue 1
Near-nanoscale-resolved energy band structure of LaNiO3/La2/3Sr1/3MnO3/SrTiO3 heterostructures and their interfaces
journal, June 2015
- Asel, Thaddeus J.; Gao, Hantian; Heinl, Tyler J.
- Journal of Vacuum Science & Technology B, Nanotechnology and Microelectronics: Materials, Processing, Measurement, and Phenomena, Vol. 33, Issue 4
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
Conductive Oxide Interfaces for Field Effect Devices
journal, June 2019
- Kornblum, Lior
- Advanced Materials Interfaces, Vol. 6, Issue 15
Coexistence of quasi-two dimensional electron and hole gas in a single tier Ca 0.5 TaO 3 /SrTiO 3 oxide heterostructure
journal, July 2019
- Pulikkotil, J. J.
- APL Materials, Vol. 7, Issue 7
Epitaxial Oxides on Semiconductors: From Fundamentals to New Devices
journal, July 2019
- Kumah, Divine P.; Ngai, Joseph H.; Kornblum, Lior
- Advanced Functional Materials
Conductive Oxide Interfaces for Field Effect Devices
journal, June 2019
- Kornblum, Lior
- Advanced Materials Interfaces, Vol. 6, Issue 15
Coexistence of quasi-two dimensional electron and hole gas in a single tier Ca 0.5 TaO 3 /SrTiO 3 oxide heterostructure
journal, July 2019
- Pulikkotil, J. J.
- APL Materials, Vol. 7, Issue 7
Interface Engineering and Emergent Phenomena in Oxide Heterostructures
journal, August 2018
- Huang, Zhen; Renshaw Wang, Xiao
- Advanced Materials, Vol. 30, Issue 47
Stimulating Oxide Heterostructures: A Review on Controlling SrTiO 3 ‐Based Heterointerfaces with External Stimuli
journal, August 2019
- Christensen, Dennis Valbjørn; Trier, Felix; Niu, Wei
- Advanced Materials Interfaces, Vol. 6, Issue 21
Formation and Tuning of 2D Electron Gas in Perovskite Heterostructures
journal, December 2019
- Maznichenko, Igor V.; Ostanin, Sergey; Ernst, Arthur
- physica status solidi (b), Vol. 257, Issue 7
Electric‐Field Control of Dirac Two‐Dimensional Electron Gas in PbTe/CdTe Heterostructures
journal, January 2019
- Zhang, Le; Shu, Tianyu; Wu, Huizhen
- physica status solidi (RRL) – Rapid Research Letters, Vol. 13, Issue 5
A termination-insensitive and robust electron gas at the heterointerface of two complex oxides
journal, September 2019
- Zhang, Meng; Du, Kai; Ren, Tianshuang
- Nature Communications, Vol. 10, Issue 1
Real-space charge-density imaging with sub-ångström resolution by four-dimensional electron microscopy
journal, October 2019
- Gao, Wenpei; Addiego, Christopher; Wang, Hui
- Nature, Vol. 575, Issue 7783
Heterogeneous integration of single-crystalline complex-oxide membranes
journal, February 2020
- Kum, Hyun S.; Lee, Hyungwoo; Kim, Sungkyu
- Nature, Vol. 578, Issue 7793
Epitaxial growth and layer-transfer techniques for heterogeneous integration of materials for electronic and photonic devices
journal, October 2019
- Kum, Hyun; Lee, Doeon; Kong, Wei
- Nature Electronics, Vol. 2, Issue 10
Strain-driven carrier-type switching of surface two-dimensional electron and hole gases in a KTaO 3 thin film
journal, January 2018
- Zhang, Xue-Jing; Liu, Bang-Gui
- Physical Chemistry Chemical Physics, Vol. 20, Issue 37
Carrier dynamics in highly excited TlInS 2 : evidence of 2D electron–hole charge separation at parallel layers
journal, January 2019
- Grivickas, Vytautas; Ščajev, Patrik; Bikbajevas, Vitalijus
- Physical Chemistry Chemical Physics, Vol. 21, Issue 4
Strain-induced indirect-to-direct bandgap transition in an np-type LaAlO 3 /SrTiO 3 (110) superlattice
journal, January 2019
- Wang, L.; Pan, W.; Hu, W. X.
- Physical Chemistry Chemical Physics, Vol. 21, Issue 13
Quantum confined two-dimensional electron/hole gas switching by facet orientation of perovskite oxides
journal, January 2018
- Zhou, Fei; Liu, Yong; Lai, Zhonghong
- RSC Advances, Vol. 8, Issue 37
Design of two-dimensional electron gas systems via polarization discontinuity from large-scale first-principles calculations
journal, January 2018
- Cheng, Jianli; Yang, Kesong
- Journal of Materials Chemistry C, Vol. 6, Issue 25
Heterointerface engineering for enhancing the electrochemical performance of solid oxide cells
journal, January 2020
- Zhao, Chenhuan; Li, Yifeng; Zhang, Wenqiang
- Energy & Environmental Science, Vol. 13, Issue 1
Two-dimensional polar metals in KNbO 3 /BaTiO 3 superlattices: first-principle calculations
journal, January 2019
- Li, Gang; Huang, Huiyu; Peng, Shaoqin
- RSC Advances, Vol. 9, Issue 61
The role of oxide interfaces in highly confined electronic and ionic conductors
journal, January 2019
- Christensen, Dennis V.; Chen, Yunzhong; Esposito, Vincenzo
- APL Materials, Vol. 7, Issue 1
Electron mobility in oxide heterostructures
journal, June 2018
- Trier, F.; Christensen, D. V.; Pryds, N.
- Journal of Physics D: Applied Physics, Vol. 51, Issue 29
Optical second harmonic generation from LaAlO 3 /SrTiO 3 interfaces with different in-plane anisotropies
journal, December 2019
- Rubano, Andrea; Scigaj, Mateusz; Sánchez, Florencio
- Journal of Physics: Condensed Matter, Vol. 32, Issue 13
A spin–orbit playground: surfaces and interfaces of transition metal oxides
journal, November 2018
- Gariglio, S.; Caviglia, A. D.; Triscone, J-M
- Reports on Progress in Physics, Vol. 82, Issue 1
Strong spin-orbit coupling and magnetism in (111)
journal, August 2018
- Bal, V. V.; Huang, Z.; Han, K.
- Physical Review B, Vol. 98, Issue 8
Theoretical prediction of Weyl fermions in the paramagnetic electride
journal, June 2019
- Liu, Liangliang; Wang, Chongze; Yi, Seho
- Physical Review B, Vol. 99, Issue 22
Influence of capping layer on the charge transport at the interfaces of (100) heterostructure
journal, November 2018
- Singh, Akhilesh Kr.; Wu, Tsung-Chi; Chen, Ming-Chin
- Physical Review Materials, Vol. 2, Issue 11
Formation of two-dimensional electron and hole gases at the interface of half-Heusler semiconductors
journal, June 2019
- Sharan, Abhishek; Gui, Zhigang; Janotti, Anderson
- Physical Review Materials, Vol. 3, Issue 6
How heteroepitaxy occurs on strontium titanate
journal, April 2019
- Cook, Seyoung; Letchworth-Weaver, Kendra; Tung, I-Cheng
- Science Advances, Vol. 5, Issue 4
A polarization-induced 2D hole gas in undoped gallium nitride quantum wells
journal, September 2019
- Chaudhuri, Reet; Bader, Samuel James; Chen, Zhen
- Science, Vol. 365, Issue 6460