journal article·2018-03Open access

Direct observation of a two-dimensional hole gas at oxide interfaces

H. Lee, N. Campbell, J. Lee, T. J. Asel, T. R. Paudel, H. Zhou, J. W. Lee, B. Noesges, J. Seo, B. Park, L. J. Brillson, S. H. Oh, E. Y. Tsymbal, M. S. Rzchowski, C. B. Eom

Nature Materials· Volume 17· Issue 3

Abstract

The discovery of a two-dimensional electron gas (2DEG) at the LaAlO3/SrTiO3 interface 1 has resulted in the observation of many properties2-5 not present in conventional semiconductor heterostructures, and so become a focal point for device applications6-8. Its counterpart, the two-dimensional hole gas (2DHG), is expected to complement the 2DEG. However, although the 2DEG has been widely observed 9 , the 2DHG has proved elusive. Herein 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. 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.
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Research context

OpenAlex topics: Electronic and Structural Properties of Oxides · Magnetic and transport properties of perovskites and related materials · Semiconductor materials and devices

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

References (43)

Show source-provided references
1. Ohtomo, A. & Hwang, H. Y. A high-mobility electron gas at the LaAlO3/SrTiO3 heterointerface. Nature 427, 423–426 (2004).10.1038/nature02308 ↗
2. Thiel, S., Hammerl, G., Schmehl, A., Schneider, C. W. & Mannhart, J. Tunable quasi-two-dimensional electron gases in oxide heterostructures. Science 313, 1942–1945 (2006).10.1126/science.1131091 ↗
3. Brinkman, A. et al. Magnetic effects at the interface between non-magnetic oxides. Nat. Mater. 6, 493–496 (2007).10.1038/nmat1931 ↗
4. Reyren, N. et al. Superconducting interfaces between insulating oxides. Science 317, 1196–1199 (2007).10.1126/science.1146006 ↗
5. Caviglia, A. D. et al. Electric field control of the LaAlO3/SrTiO3 interface ground state. Nature 456, 624–627 (2008).10.1038/nature07576 ↗
6. Mannhart, J. & Schlom, D. G. Oxide interfaces—an opportunity for electronics. Science 327, 1607–1611 (2010).10.1126/science.1181862 ↗
7. Cheng, G. L. et al. Sketched oxide single-electron transistor. Nat. Nanotech. 6, 343–347 (2011).10.1038/nnano.2011.56 ↗
8. Lesne, E. et al. Highly efficient and tunable spin-to-charge conversion through Rashba coupling at oxide interfaces. Nat. Mater. 15, 1261–1266 (2016).10.1038/nmat4726 ↗
9. Mannhart, J., Blank, D. H. A., Hwang, H. Y., Millis, A. J. & Triscone, J. M. Two-dimensional electron gases at oxide interfaces. MRS Bull. 33, 1027–1034 (2008).10.1557/mrs2008.222 ↗
10. Nakagawa, N., Hwang, H. Y. & Muller, D. A. Why some interfaces cannot be sharp. Nat. Mater. 5, 204–209 (2006).10.1038/nmat1569 ↗
11. Huijben, M. et al. Electronically coupled complementary interfaces between perovskite band insulators. Nat. Mater. 5, 556–560 (2006).10.1038/nmat1675 ↗
12. Herranz, G. et al. High mobility in LaAlO3/SrTiO3 heterostructures: origin, dimensionality, and perspectives. Phys. Rev. Lett. 98, 216803 (2007).10.1103/PhysRevLett.98.216803 ↗
13. Hwang, H. Y. et al. Emergent phenomena at oxide interfaces. Nat. Mater. 11, 103–113 (2012).10.1038/nmat3223 ↗
14. Chen, Y. Z. et al. Extreme mobility enhancement of two-dimensional electron gases at oxide interfaces by charge-transfer-induced modulation doping. Nat. Mater. 14, 801–806 (2015).10.1038/nmat4303 ↗
15. Pentcheva, R. & Pickett, W. E. Charge localization or itineracy at LaAlO3/SrTiO3 interfaces: hole polarons, oxygen vacancies, and mobile electrons. Phys. Rev. B 74, 035112 (2006).10.1103/PhysRevB.74.035112 ↗
16. Park, M. S., Rhim, S. H. & Freeman, A. J. Charge compensation and mixed valency in LaAlO3/SrTiO3 heterointerfaces studied by the FLAPW method. Phys. Rev. B 74, 205416 (2006).
17. Pentcheva, R. et al. Parallel electron–hole bilayer conductivity from electronic interface reconstruction. Phys. Rev. Lett. 104, 166804 (2010).10.1103/PhysRevLett.104.166804 ↗
18. Huijben, M. et al. Local probing of coupled interfaces between two-dimensional electron and hole gases in oxide heterostructures by variable-temperature scanning tunneling spectroscopy. Phys. Rev. B 86, 035140 (2012).10.1103/PhysRevB.86.035140 ↗
19. Zhong, Z. C., Xu, P. X. & Kelly, P. J. Polarity-induced oxygen vacancies at LaAlO3/SrTiO3 interfaces. Phys. Rev. B 82, 165127 (2010).10.1103/PhysRevB.82.165127 ↗
20. Rubano, A. et al. Influence of atomic termination on the LaAlO3/SrTiO3 interfacial polar rearrangement. Phys. Rev. B 88, 035405 (2013).
21. Cancellieri, C. et al. Polaronic metal state at the LaAlO3/SrTiO3 interface. Nat. Commun. 7, 10386 (2016).
22. Luo, W. D., Duan, W. H., Louie, S. G. & Cohen, M. L. Structural and electronic properties of n-doped and p-doped SrTiO3. Phys. Rev. B 70, 214109 (2004).
23. Himmetoglu, B., Janotti, A., Peelaers, H., Alkauskas, A. & Van de Walle, C. G. First-principles study of the mobility of SrTiO3. Phys. Rev. B 90, 241204 (2014).
24. Koch, C. T. A flux-preserving non-linear inline holography reconstruction algorithm for partially coherent electrons. Ultramicroscopy 108, 141–150 (2008).10.1016/j.ultramic.2007.03.007 ↗
25. Muller, D. A., Nakagawa, N., Ohtomo, A., Grazul, J. L. & Hwang, H. Y. Atomic-scale imaging of nanoengineered oxygen vacancy profiles in SrTiO3. Nature 430, 657–661 (2004).10.1038/nature02756 ↗
26. Caviglia, A. D. et al. Tunable Rashba spin–orbit interaction at oxide interfaces. Phys. Rev. Lett. 104, 126803 (2010).10.1103/PhysRevLett.104.126803 ↗
27. Millis, A. J. & Schlom, D. G. Electron–hole liquids in transition-metal oxide heterostructures. Phys. Rev. B 82, 073101 (2010).10.1103/PhysRevB.82.073101 ↗
28. Szymanska, M. H. & Littlewood, P. B. Excitonic binding in coupled quantum wells. Phys. Rev. B 67, 193305 (2003).10.1103/PhysRevB.67.193305 ↗
29. Tse, W. K. & Das Sarma, S. Coulomb drag and spin drag in the presence of spin–orbit coupling. Phys. Rev. B 75, 045333 (2007).
30. Eisenstein, J. P. & MacDonald, A. H. Bose–Einstein condensation of excitons in bilayer electron systems. Nature 432, 691–694 (2004).10.1038/nature03081 ↗
31. Bark, C. W. et al. Tailoring a two-dimensional electron gas at the LaAlO3/SrTiO3 (001) interface by epitaxial strain. Proc. Natl Acad. Sci. USA 108, 4720–4724 (2011).10.1073/pnas.1014849108 ↗
32. Bi, F. et al. Room-temperature electronically-controlled ferromagnetism at the LaAlO3/SrTiO3 interface. Nat. Commun. 5, 5019 (2014).
33. Blochl, P. E. Projector augmented-wave method. Phys. Rev. B 50, 17953–17979 (1994).10.1103/PhysRevB.50.17953 ↗
34. Kresse, G. & Furthmuller, J. Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. Phys. Rev. B 54, 11169–11186 (1996).10.1103/PhysRevB.54.11169 ↗
35. Kresse, G. & Joubert, D. From ultrasoft pseudopotentials to the projector augmented-wave method. Phys. Rev. B 59, 1758–1775 (1999).10.1103/PhysRevB.59.1758 ↗
36. Zhou, H. et al. Anomalous expansion of the copper–apical-oxygen distance in superconducting cuprate bilayers. Proc. Natl Acad. Sci. USA 107, 8103–8107 (2010).10.1073/pnas.0914702107 ↗
37. Zhou, H., Pindak, R., Clarke, R., Steinberg, D. M. & Yacoby, Y. The limits of ultrahigh-resolution X-ray mapping: estimating uncertainties in thin-film and interface structures determined by phase retrieval methods. J. Phys. D. 45, 195302 (2012).
38. Koch, C. T. Towards full-resolution inline electron holography. Micron 63, 69–75 (2014).10.1016/j.micron.2013.10.009 ↗
39. Janolin, P. E. Strain on ferroelectric thin films. J. Mater. Sci. 44, 5025–5048 (2009).10.1007/s10853-009-3553-1 ↗
40. Zhang, J. et al. Depth-resolved subsurface defects in chemically etched SrTiO3. Appl. Phys. Lett. 94, 092904 (2009).
41. Brillson, L. J. Applications of depth-resolved cathodoluminescence spectroscopy. J. Phys. D. 45, 183001 (2012).10.1088/0022-3727/45/18/183001 ↗
42. Asel, T. J. et al. Near-nanoscale-resolved energy band structure of LaNiO3/La2/3Sr1/3MnO3/SrTiO3 heterostructures and their interfaces. J. Vac. Sci. Technol. B 33, 04E103 (2015).
43. Rutkowski, M. M., McNicholas, K., Zeng, Z. Q., Tuomisto, F. & Brillson, L. J. Optical identification of oxygen vacancy formation at SrTiO3–(Ba,Sr)TiO3 heterostructures. J. Phys. D. 47, 255303 (2014).10.1088/0022-3727/47/25/255303 ↗