Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

  • Letter
  • Published:

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 interface1 has resulted in the observation of many properties2,3,4,5 not present in conventional semiconductor heterostructures, and so become a focal point for device applications6,7,8. Its counterpart, the two-dimensional hole gas (2DHG), is expected to complement the 2DEG. However, although the 2DEG has been widely observed9, 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.

This is a preview of subscription content, access via your institution

Access options

Buy this article

Prices may be subject to local taxes which are calculated during checkout

Fig. 1: Atomically abrupt p-type interface in epitaxially grown STO/LAO/STO heterostructure.
Fig. 2: Electrical transport properties of the top and bottom interfaces in the STO/LAO/STO heterostructure.
Fig. 3: Charge distribution in the STO/LAO/STO heterostructure.
Fig. 4: Oxygen-vacancy distribution in the STO/LAO/STO heterostructure.

Similar content being viewed by others

References

  1. Ohtomo, A. & Hwang, H. Y. A high-mobility electron gas at the LaAlO3/SrTiO3 heterointerface. Nature 427, 423–426 (2004).

    CAS  Google Scholar 

  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).

    CAS  Google Scholar 

  3. Brinkman, A. et al. Magnetic effects at the interface between non-magnetic oxides. Nat. Mater. 6, 493–496 (2007).

    CAS  Google Scholar 

  4. Reyren, N. et al. Superconducting interfaces between insulating oxides. Science 317, 1196–1199 (2007).

    CAS  Google Scholar 

  5. Caviglia, A. D. et al. Electric field control of the LaAlO3/SrTiO3 interface ground state. Nature 456, 624–627 (2008).

    CAS  Google Scholar 

  6. Mannhart, J. & Schlom, D. G. Oxide interfaces—an opportunity for electronics. Science 327, 1607–1611 (2010).

    CAS  Google Scholar 

  7. Cheng, G. L. et al. Sketched oxide single-electron transistor. Nat. Nanotech. 6, 343–347 (2011).

    CAS  Google Scholar 

  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).

    CAS  Google Scholar 

  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).

    CAS  Google Scholar 

  10. Nakagawa, N., Hwang, H. Y. & Muller, D. A. Why some interfaces cannot be sharp. Nat. Mater. 5, 204–209 (2006).

    CAS  Google Scholar 

  11. Huijben, M. et al. Electronically coupled complementary interfaces between perovskite band insulators. Nat. Mater. 5, 556–560 (2006).

    CAS  Google Scholar 

  12. Herranz, G. et al. High mobility in LaAlO3/SrTiO3 heterostructures: origin, dimensionality, and perspectives. Phys. Rev. Lett. 98, 216803 (2007).

    CAS  Google Scholar 

  13. Hwang, H. Y. et al. Emergent phenomena at oxide interfaces. Nat. Mater. 11, 103–113 (2012).

    CAS  Google Scholar 

  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).

    CAS  Google Scholar 

  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).

    Google Scholar 

  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).

    Google Scholar 

  17. Pentcheva, R. et al. Parallel electron–hole bilayer conductivity from electronic interface reconstruction. Phys. Rev. Lett. 104, 166804 (2010).

    CAS  Google Scholar 

  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).

    Google Scholar 

  19. Zhong, Z. C., Xu, P. X. & Kelly, P. J. Polarity-induced oxygen vacancies at LaAlO3/SrTiO3 interfaces. Phys. Rev. B 82, 165127 (2010).

    Google Scholar 

  20. Rubano, A. et al. Influence of atomic termination on the LaAlO3/SrTiO3 interfacial polar rearrangement. Phys. Rev. B 88, 035405 (2013).

    Google Scholar 

  21. Cancellieri, C. et al. Polaronic metal state at the LaAlO3/SrTiO3 interface. Nat. Commun. 7, 10386 (2016).

    CAS  Google Scholar 

  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).

    Google Scholar 

  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).

    Google Scholar 

  24. Koch, C. T. A flux-preserving non-linear inline holography reconstruction algorithm for partially coherent electrons. Ultramicroscopy 108, 141–150 (2008).

    CAS  Google Scholar 

  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).

    CAS  Google Scholar 

  26. Caviglia, A. D. et al. Tunable Rashba spin–orbit interaction at oxide interfaces. Phys. Rev. Lett. 104, 126803 (2010).

    CAS  Google Scholar 

  27. Millis, A. J. & Schlom, D. G. Electron–hole liquids in transition-metal oxide heterostructures. Phys. Rev. B 82, 073101 (2010).

    Google Scholar 

  28. Szymanska, M. H. & Littlewood, P. B. Excitonic binding in coupled quantum wells. Phys. Rev. B 67, 193305 (2003).

    Google Scholar 

  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).

    Google Scholar 

  30. Eisenstein, J. P. & MacDonald, A. H. Bose–Einstein condensation of excitons in bilayer electron systems. Nature 432, 691–694 (2004).

    CAS  Google Scholar 

  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).

    CAS  Google Scholar 

  32. Bi, F. et al. Room-temperature electronically-controlled ferromagnetism at the LaAlO3/SrTiO3 interface. Nat. Commun. 5, 5019 (2014).

    CAS  Google Scholar 

  33. Blochl, P. E. Projector augmented-wave method. Phys. Rev. B 50, 17953–17979 (1994).

    CAS  Google Scholar 

  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).

    CAS  Google Scholar 

  35. Kresse, G. & Joubert, D. From ultrasoft pseudopotentials to the projector augmented-wave method. Phys. Rev. B 59, 1758–1775 (1999).

    CAS  Google Scholar 

  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).

    CAS  Google Scholar 

  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).

    Google Scholar 

  38. Koch, C. T. Towards full-resolution inline electron holography. Micron 63, 69–75 (2014).

    Google Scholar 

  39. Janolin, P. E. Strain on ferroelectric thin films. J. Mater. Sci. 44, 5025–5048 (2009).

    CAS  Google Scholar 

  40. Zhang, J. et al. Depth-resolved subsurface defects in chemically etched SrTiO3. Appl. Phys. Lett. 94, 092904 (2009).

    Google Scholar 

  41. Brillson, L. J. Applications of depth-resolved cathodoluminescence spectroscopy. J. Phys. D. 45, 183001 (2012).

    Google Scholar 

  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).

    Google Scholar 

  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).

    Google Scholar 

Download references

Acknowledgements

This work was supported by the National Science Foundation (NSF) under DMREF Grant number DMR-1629270, AFOSR under award number FA9550-15-1-0334 and AOARD under award number FA2386-15-1-4046. Transport measurement at the University of Wisconsin-Madison was supported by the US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, under award number DE-FG02-06ER46327. Research at the University of Nebraska-Lincoln was supported by the NSF MRSEC (Grant no. DMR-1420645). T.J.A. and L.J.B. acknowledge support from NSF grant DMR 1305193. Use of the Advanced Photon Source was supported by the US DOE, Office of Science, Office of Basic Energy Sciences, under Contract no. DE-AC02-06CH11357. STEM and in-line electron holography works by S.H.O. were supported by the Creative Materials Discovery Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science, ICT and Future Planning (NRF-2015M3D1A1070672) and NRF grant funded by the Korea government (NRF-2015R1A2A2A01007904).

Author information

Authors and Affiliations

Authors

Contributions

H.L. and C.B.E. conceived the project. C.B.E., M.S.R., E.Y.T., S.H.O. and L.J.B. supervised the experiments. H.L., J.W.L. and C.B.E. fabricated and characterized the thin-film samples. N.C. and M.S.R. carried out the electrical transport measurements. J.L., B.P., J.S. and S.H.O. carried out the STEM and in-line holography measurements. T.J.A. and B.N. performed the DR-CLS measurements. T.R.P. and E.Y.T. performed the theoretical calculations. H.Z. performed the synchrotron diffraction measurements. H.L., N.C., J.L., T.A., T.R.P., H.Z. and C.B.E. prepared the manuscript. C.B.E. directed the overall research.

Corresponding author

Correspondence to C. B. Eom.

Ethics declarations

Competing interests

The authors declare no competing financial interests.

Additional information

Publisher’s note: Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary information

Supplementary Information

Supplementary Information.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Lee, H., Campbell, N., Lee, J. et al. Direct observation of a two-dimensional hole gas at oxide interfaces. Nature Mater 17, 231–236 (2018). https://doi.org/10.1038/s41563-017-0002-4

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/s41563-017-0002-4

This article is cited by

Search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing