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.

  • Article
  • Published:

Extreme mobility enhancement of two-dimensional electron gases at oxide interfaces by charge-transfer-induced modulation doping

Abstract

Two-dimensional electron gases (2DEGs) formed at the interface of insulating complex oxides promise the development of all-oxide electronic devices. These 2DEGs involve many-body interactions that give rise to a variety of physical phenomena such as superconductivity, magnetism, tunable metal–insulator transitions and phase separation. Increasing the mobility of the 2DEG, however, remains a major challenge. Here, we show that the electron mobility is enhanced by more than two orders of magnitude by inserting a single-unit-cell insulating layer of polar La1−xSrxMnO3 (x = 0, 1/8, and 1/3) at the interface between disordered LaAlO3 and crystalline SrTiO3 produced at room temperature. Resonant X-ray spectroscopy and transmission electron microscopy show that the manganite layer undergoes unambiguous electronic reconstruction, leading to modulation doping of such atomically engineered complex oxide heterointerfaces. At low temperatures, the modulation-doped 2DEG exhibits Shubnikov–de Haas oscillations and fingerprints of the quantum Hall effect, demonstrating unprecedented high mobility and low electron density.

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

Figure 1: Atomically engineered complex oxide interfaces with a single-unit-cell manganite buffer layer.
Figure 2: Electronic properties of d-LAO (8.5 nm)/STO heterostructures with and without LSMO (x = 0, 1/8, and 1/3) buffer layers.
Figure 3: Electronic reconstructions in d-LAO/STO heterostructures.
Figure 4: Modulation doping of STO-based heterostructures.
Figure 5: Quantum oscillations at modulation-doped oxide interfaces.

Similar content being viewed by others

References

  1. Kroemer, H. Nobel Lecture: Quasielectric fields and band offsets: Teaching electrons new tricks. Rev. Mod. Phys. 73, 783–793 (2001).

    Article  CAS  Google Scholar 

  2. Schlom, D. G. & Pfeiffer, L. N. Oxide electronics: Upward mobility rocks! Nature Mater. 9, 881–883 (2010).

    Article  CAS  Google Scholar 

  3. Dingle, R., Stormer, H. L., Gossard, A. C. & Wiegmann, W. Electron mobilities in modulation-doped semiconductor heterojunction superlattices. Appl. Phys. Lett. 33, 665–667 (1978).

    Article  CAS  Google Scholar 

  4. Tsui, D. C., Stormer, H. L. & Gossard, A. C. Two-dimensional magnetotransport in the extreme quantum limit. Phys. Rev. Lett. 48, 1559–1562 (1982).

    Article  CAS  Google Scholar 

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

    Article  CAS  Google Scholar 

  6. Chen, Y. Z. et al. A high-mobility two-dimensional electron gas at the spinel/perovskite interface of γ-Al2O3/SrTiO3 . Nature Commun. 4, 1371 (2013).

    Article  CAS  Google Scholar 

  7. Mannhart, J. & Schlom, D. G. Oxide interfaces: An opportunity for electronics. Science 327, 1607–1611 (2010).

    Article  CAS  Google Scholar 

  8. Miletto Granozio, F., Koster, G. & Rijnders, G. Functional oxide interfaces. Mater. Res. Soc. Bull. 38, 1017–1023 (2013).

    Article  Google Scholar 

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

    Article  CAS  Google Scholar 

  10. Stemmer, S. & Allen, S. J. Two-dimensional electron gases at complex oxide interfaces. Annu. Rev. Mater. Sci. 44, 151–171 (2014).

    Article  CAS  Google Scholar 

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

    Article  CAS  Google Scholar 

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

    Article  CAS  Google Scholar 

  13. Lee, J-S. et al. Titanium d xy ferromagnetism at the LaAlO3/SrTiO3 interface. Nature Mater. 12, 703–706 (2013).

    Article  CAS  Google Scholar 

  14. Cen, C. et al. Nanoscale control of an interfacial metal–insulator transition at room temperature. Nature Mater. 7, 298–302 (2008).

    Article  CAS  Google Scholar 

  15. Ariando, et al. Electronic phase separation at the LaAlO3/SrTiO3 interface. Nature Commun. 2, 188 (2011).

    Article  CAS  Google Scholar 

  16. Huijben, M. et al. Defect engineering in oxide heterostructures by enhanced oxygen surface exchange. Adv. Funct. Mater. 23, 5240–5248 (2013).

    Article  CAS  Google Scholar 

  17. Caviglia, A. D. et al. Two-dimensional quantum oscillations of the conductance at LaAlO3/SrTiO3 interfaces. Phys. Rev. Lett. 105, 236802 (2010).

    Article  CAS  Google Scholar 

  18. Xie, Y. W., Bell, C., Hikita, Y., Harashima, S. & Hwang, H. Y. Enhancing electron mobility at the LaAlO3/SrTiO3 interface by surface control. Adv. Mater. 25, 4735–4738 (2013).

    Article  CAS  Google Scholar 

  19. Chen, Y. Z. et al. Room temperature formation of high-mobility two-dimensional electron gases at crystalline complex oxide interfaces. Adv. Mater. 26, 1462–1467 (2014).

    Article  CAS  Google Scholar 

  20. Hesper, R., Tjeng, L. H., Heeres, A. & Sawatzky, G. A. Photoemission evidence of electronic stabilization of polar surfaces in K3C60. Phys. Rev. B 62, 16046 (2000).

    Article  CAS  Google Scholar 

  21. Jang, H. W. et al. Metallic and insulating oxide interfaces controlled by electronic correlations. Science 331, 886–889 (2011).

    Article  CAS  Google Scholar 

  22. Chambers, S. A. et al. Instability, intermixing and electronic structure at the epitaxial LaAlO3/SrTiO3(001) heterojunction. Surf. Sci. Rep. 65, 317–352 (2010).

    Article  CAS  Google Scholar 

  23. Kalabukhov, A. et al. Effect of oxygen vacancies in the SrTiO3 substrate on the electrical properties of the LaAlO3/SrTiO3 interface. Phys. Rev. B 75, 121404(R) (2007).

    Article  Google Scholar 

  24. Chen, Y. Z. et al. Metallic and insulating interfaces of amorphous SrTiO3-based oxide heterostructures. Nano Lett. 11, 3774–3778 (2011).

    Article  CAS  Google Scholar 

  25. Christensen, D. V. et al. Controlling interfacial states in amorphous/crystalline LaAlO3/SrTiO3 heterostructures by electric fields. Appl. Phys. Lett. 102, 021602 (2013).

    Article  Google Scholar 

  26. Chen, Y. Z., Pryds, N., Sun, J. R., Shen, B. G. & Linderoth, S. High-mobility two-dimensional electron gases at oxide interfaces: Origins and opportunities. Chin. Phys. B 22, 116803 (2013).

    Article  Google Scholar 

  27. Gabay, M. Triscone, J-M. Oxide heterostructures: Hund rules with a twist. Nature Phys. 9, 610–611 (2013).

    Article  CAS  Google Scholar 

  28. Delugas, P. et al. Spontaneous 2-dimensional carrier confinement at the n-type SrTiO3/LaAlO3 interface. Phys. Rev. Lett. 106, 166807 (2011).

    Article  Google Scholar 

  29. Son, W. J., Cho, E., Lee, B., Lee, J. & Han, S. Density and spatial distribution of charge carriers in the intrinsic n-type LaAlO3-SrTiO3 interface. Phys. Rev. B 79, 245411 (2009).

    Article  Google Scholar 

  30. Berner, G. et al. Direct k-space mapping of the electronic structure in an oxide–oxide interface. Phys. Rev. Lett. 110, 247601 (2013).

    Article  CAS  Google Scholar 

  31. Huijben, M. et al. Critical thickness and orbital ordering in ultrathin La0.7Sr0.3MnO3 films. Phys. Rev. B 78, 094413 (2008).

    Article  Google Scholar 

  32. Shibuya, K., Ohnishi, T., Lippmaa, M., Kawasaki, M. & Koinuma, H. Single crystal SrTiO3 field-effect transistor with an atomically flat amorphous CaHfO3 gate insulator. Appl. Phys. Lett. 85, 425–427 (2004).

    Article  CAS  Google Scholar 

  33. Cen, C., Thiel, S., Mannhart, J. & Levy, J. Oxide nanoelectronics on demand. Science 323, 1026–1030 (2009).

    Article  CAS  Google Scholar 

  34. Mkhoyan, K. A., Maccagnano–Zacher, S. E., Kirkland, E. J. & Silcox, J. Effects of amorphous layers on ADF-STEM imaging. Ultramicroscopy 108, 791–803 (2008).

    Article  CAS  Google Scholar 

  35. Van Aert, S., Chang, L. Y., Bals, S., Kirkland, A. I. & Van Tendeloo, G. Effect of amorphous layers on the interpretation of restored exit waves. Ultramicroscopy 109, 237–246 (2009).

    Article  CAS  Google Scholar 

  36. Cancellieri, C. et al. Interface Fermi states of LaAlO3/SrTiO3 and related heterostructures. Phys. Rev. Lett. 110, 137601 (2013).

    Article  CAS  Google Scholar 

  37. Haverkort, M. W., Zwierzycki, M. & Andersen, O. K. Multiplet ligand-field theory using Wannier orbitals. Phys. Rev. B 85, 165113 (2012).

    Article  Google Scholar 

  38. Wachtel, E. & Lubomirsky, I. Quasi-amorphous inorganic thin films: Non-crystalline polar phases. Adv. Mater. 22, 2485–2493 (2010).

    Article  CAS  Google Scholar 

  39. Ferguson, J. D. et al. Epitaxial oxygen getter for a brownmillerite phase transformation in manganite films. Adv. Mater. 23, 1226–1230 (2011).

    Article  CAS  Google Scholar 

  40. Jung, J. H. et al. Determination of electronic band structures of CaMnO3 and LaMnO3 using optical-conductivity analyses. Phys. Rev. B 55, 15489 (1997).

    Article  CAS  Google Scholar 

  41. Sawa, A. et al. Fermi level shift in La1−xSrxMO3 (M = Mn, Fe, Co, and Ni) probed by Schottky-like heteroepitaxial junctions with SrTi0.99Nb0.01O3 . Appl. Phys. Lett. 90, 252102 (2007).

    Article  Google Scholar 

  42. Chen, Y. Z. et al. Charge ordering transition near the interface of the (011)-oriented La1−xSrxMnO3 (x 1/8) films. Appl. Phys. Lett. 93, 152515 (2008).

    Article  Google Scholar 

  43. Shubnikov, L. W. & de Haas, W. J. Magnetische Widerstandsvergrösserung in Einkristallen von Wismut bei tiefen Temperaturen. Proc. R Neth. Acad. Arts Sci. 33, 130–133 (1930).

    CAS  Google Scholar 

  44. Son, J. et al. Epitaxial SrTiO3 films with electron mobilities exceeding 30,000 cm2 V−1 s−1. Nature Mater. 9, 482–484 (2010).

    Article  CAS  Google Scholar 

  45. Klitzing, K. v., Dorda, G. & Pepper, M. New methods for high-accuracy determination of the fine-structure constant based on quantized Hall resistance. Phys. Rev. Lett. 45, 494–497 (1980).

    Article  Google Scholar 

  46. Trier, F. et al. Quantum Hall effect at a SrTiO3-based heterointerface: Evidence of a multiple quantum well nature (in the press).

  47. Burnus, T. et al. Local electronic structure and magnetic properties of LaMn0.5Co0.5O3 studied by x-ray absorption and magnetic circular dichroism spectroscopy. Phys. Rev. B 77, 125124 (2008).

    Article  Google Scholar 

  48. Watanabe, M., Okunishi, E. & Ishizuka, K. Analysis of spectrum-imaging datasets in atomic-resolution electron microscopy. Microsc. Anal. 23, 5–7 (2009).

    Google Scholar 

  49. Keenan, M. R. & Kotula, P. G. Accounting for poisson noise in the multivariate analysis of ToF-SIMS spectrum images. Surf. Interface Anal. 36, 203–212 (2004).

    Article  CAS  Google Scholar 

  50. Hawthorn, D. G. et al. An in-vacuum diffractometer for resonant elastic soft x-ray scattering. Rev. Sci. Instrum. 82, 073104 (2011).

    Article  CAS  Google Scholar 

Download references

Acknowledgements

The authors gratefully acknowledge discussions with J. Mannhart, J. R. Sun and B. G. Shen, and technical assistance from J. Geyti, L. Han, K. V. Hansen, S. Upadhyay, C. Olsen and A. Jellinggaard. This work was funded by the European Union (EU) Council under the 7th Framework Program (FP7) grant number NMP3-LA-2010-246102 IFOX, by funding from the European Research Council (ERC) under FP7, ERC grant No. 246791—COUNTATOMS and ERC Starting Grant 278510 VORTEX. The Qu-Ant-EM microscope was partly funded by the Hercules Fund from the Flemish Government. The authors acknowledge also financial support from EU under FP7 under a contract for an Integrated Infrastructure Initiative. Reference No. 312483-ESTEEM2. Funding from the Fund for Scientific Research Flanders is acknowledged for FWO project G.0044.13N (‘Charge ordering’). Funding from the Danish Agency for Science, Technology and Innovation, and the Lundbeck Foundation are acknowledged. The Center for Quantum Devices is supported by the Danish National Research Foundation. The Canadian work was supported by NSERC and the Max Planck-UBC Centre for Quantum Materials. Some experiments for this work were performed at the Canadian Light Source, which is funded by the Canada Foundation for Innovation, NSERC, the National Research Council of Canada, the Canadian Institutes of Health Research, the Government of Saskatchewan, Western Economic Diversification Canada, and the University of Saskatchewan.

Author information

Authors and Affiliations

Authors

Contributions

Y.Z.C.: concept design, film growth, transport measurements, data analysis, interpretation and writing of the manuscript. The contributions of other authors are as follows. Transport measurements and analysis: D.V.C., N.H.A., M.Huijben, J.A.S., M.Honig and S.I.; STEM and EELS measurements and analysis: N.G., R.E., J.V. and G.V.T.; XPS measurements and analysis: T.W., G.K., M.Huijben, G.R. and N.B.; RXR measurements and analysis: R.J.G., S.M., F.H., R.S. and G.A.S.; SdH measurements: F.T., G.E.D.K.P. and T.S.J.; Data discussion: N.P. and S.L. All authors extensively discussed the results and the manuscript.

Corresponding author

Correspondence to Y. Z. Chen.

Ethics declarations

Competing interests

The authors declare no competing financial interests.

Supplementary information

Supplementary Information

Supplementary Information (PDF 1278 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Chen, Y., Trier, F., Wijnands, T. et al. Extreme mobility enhancement of two-dimensional electron gases at oxide interfaces by charge-transfer-induced modulation doping. Nature Mater 14, 801–806 (2015). https://doi.org/10.1038/nmat4303

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/nmat4303

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