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:

Graphene-assisted spontaneous relaxation towards dislocation-free heteroepitaxy

Nature Nanotechnology volume 15, pages 272–276 (2020)Cite this article

Subjects

Abstract

Although conventional homoepitaxy forms high-quality epitaxial layers1,2,3,4,5, the limited set of material systems for commercially available wafers restricts the range of materials that can be grown homoepitaxially. At the same time, conventional heteroepitaxy of lattice-mismatched systems produces dislocations above a critical strain energy to release the accumulated strain energy as the film thickness increases. The formation of dislocations, which severely degrade electronic/photonic device performances6,7,8, is fundamentally unavoidable in highly lattice-mismatched epitaxy9,10,11. Here, we introduce a unique mechanism of relaxing misfit strain in heteroepitaxial films that can enable effective lattice engineering. We have observed that heteroepitaxy on graphene-coated substrates allows for spontaneous relaxation of misfit strain owing to the slippery graphene surface while achieving single-crystalline films by reading the atomic potential from the substrate. This spontaneous relaxation technique could transform the monolithic integration of largely lattice-mismatched systems by covering a wide range of the misfit spectrum to enhance and broaden the functionality of semiconductor devices for advanced electronics and photonics.

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

Access options

Buy this article

  • Purchase on Springer Link
  • Instant access to full article PDF
Buy now

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

Fig. 1: Strain analysis by Raman spectra and schematic images.
Fig. 2: Cross-sectional ADF-STEM images of InGaP grown on bare GaAs and graphene/GaAs.
Fig. 3: Theoretical calculation to understand spontaneous relaxation.
Fig. 4: Highly mismatched system of GaP on GaAs.

Similar content being viewed by others

Data availability

The data that support the findings of this study are available from the corresponding author upon reasonable request.

References

  1. Chen, C. Q. et al. GaN homoepitaxy on freestanding (1100) oriented GaN substrates. Appl. Phys. Lett. 81, 3194–3196 (2002).

    Article  CAS  Google Scholar 

  2. Kwon, O. et al. Monolithic integration of AlGaInP laser diodes on SiGe/Si substrates by molecular beam epitaxy. J. Appl. Phys. 100, 13103 (2006).

    Article  Google Scholar 

  3. Matsunami, H. & Kimoto, T. Step-controlled epitaxial growth of SiC: high quality homoepitaxy. Mater. Sci. Eng. R. Rep. 20, 125–166 (1997).

    Article  Google Scholar 

  4. Vaisman, M. et al. Effects of growth temperature and device structure on GaP solar cells grown by molecular beam epitaxy. Appl. Phys. Lett. 106, 063903 (2015).

    Article  Google Scholar 

  5. Voigtländer, B., Weber, T., Šmilauer, P. & Wolf, D. E. Transition from island growth to step-flow growth for Si/Si (100) epitaxy. Phys. Rev. Lett. 78, 2164–2167 (1997).

    Article  Google Scholar 

  6. Luan, H.-C. et al. High-quality Ge epilayers on Si with low threading-dislocation densities. Appl. Phys. Lett. 75, 2909–2911 (1999).

    Article  CAS  Google Scholar 

  7. Currie, M. T., Samavedam, S. B., Langdo, T. A., Leitz, C. W. & Fitzgerald, E. A. Controlling threading dislocation densities in Ge on Si using graded SiGe layers and chemical-mechanical polishing. Appl. Phys. Lett. 72, 1718–1720 (1998).

    Article  CAS  Google Scholar 

  8. Andre, C. L. et al. Impact of dislocation densities on n+∕ p and p+∕ n junction GaAs diodes and solar cells on SiGe virtual substrates. J. Appl. Phys. 98, 14502 (2005).

    Article  Google Scholar 

  9. Lee, M. L., Antoniadis, D. A. & Fitzgerald, E. A. Challenges in epitaxial growth of SiGe buffers on Si (111), (110), and (112). Thin Solid Films 508, 136–139 (2006).

    Article  CAS  Google Scholar 

  10. Chen, R. et al. Nanolasers grown on silicon. Nat. Photonics 5, 170–175 (2011).

    Article  CAS  Google Scholar 

  11. Ebert, C. B., Eyres, L. A., Fejer, M. M. & Harris, J. S. Jr MBE growth of antiphase GaAs films using GaAs/Ge/GaAs heteroepitaxy. J. Cryst. Growth 201-202, 187–193 (1999).

    Article  Google Scholar 

  12. Lee, M. L., Fitzgerald, E. A., Bulsara, M. T., Currie, M. T. & Lochtefeld, A. Strained Si, SiGe, and Ge channels for high-mobility metal-oxide-semiconductor field-effect transistors. J. Appl. Phys. 97, 1 (2005).

    Article  Google Scholar 

  13. Bean, J. C., Sheng, T. T., Feldman, L. C., Fiory, A. T. & Lynch, R. T. Pseudomorphic growth of GexSi1−x on silicon by molecular beam epitaxy. Appl. Phys. Lett. 44, 102–104 (1984).

    Article  CAS  Google Scholar 

  14. Fitzgerald, E. A. et al. Totally relaxed GexSi1−x layers with low threading dislocation densities grown on Si substrates. Appl. Phys. Lett. 59, 811–813 (1991).

    Article  CAS  Google Scholar 

  15. Song, T. L., Chua, S. J., Fitzgerald, E. A., Chen, P. & Tripathy, S. Strain relaxation in graded InGaN/GaN epilayers grown on sapphire. Appl. Phys. Lett. 83, 1545–1547 (2003).

    Article  CAS  Google Scholar 

  16. Massies, J. & Grandjean, N. Oscillation of the lattice relaxation in layer-by-layer epitaxial growth of highly strained materials. Phys. Rev. Lett. 71, 1411–1414 (1993).

    Article  CAS  Google Scholar 

  17. Daruka, I. & Barabási, A.-L. Dislocation-free island formation in heteroepitaxial growth: a study at equilibrium. Phys. Rev. Lett. 79, 3708–3711 (1997).

    Article  CAS  Google Scholar 

  18. Kim, Y. et al. Remote epitaxy through graphene enables two-dimensional material-based layer transfer. Nature 544, 340–343 (2017).

    Article  CAS  Google Scholar 

  19. Kong, W. et al. Polarity governs atomic interaction through two-dimensional materials. Nat. Mater. 17, 999–1004 (2018).

    Article  CAS  Google Scholar 

  20. Li, X. et al. Large-area two-dimensional layered hexagonal boron nitride grown on sapphire by metalorganic vapor phase epitaxy. Cryst. Growth Des. 16, 3409–3415 (2016).

    Article  CAS  Google Scholar 

  21. Attolini, G. et al. Optical and structural characterization of LP MOVPE grown lattice matched InGaP/GaAs heterostructures. Mater. Sci. Eng. B 91-92, 123–127 (2002).

    Article  Google Scholar 

  22. Kato, T., Matsumoto, T. & Ishida, T. Raman spectral behavior of In1-xGaxP (0 < x < 1). Jpn. J. Appl. Phys. 27, 983–986 (1988).

    Article  CAS  Google Scholar 

  23. Lee, H. et al. Study of strain and disorder of InxGa1−xP/(GaAs, graded GaP)(0.25 ≤ x ≤ 0.8) using spectroscopic ellipsometry and Raman spectroscopy. J. Appl. Phys. 75, 5040–5051 (1994).

    Article  CAS  Google Scholar 

  24. King-Ning, T., Mayer, J. W. & Feldman, L. C. Electronic Thin Film Science for Electrical Engineers and Materials Scientists (Macmillan, 1996).

  25. Matthews, J. W. & Blakeslee, A. E. Defects in epitaxial multilayers: I. Misfit dislocations. J. Cryst. Growth 27, 118–125 (1974).

    CAS  Google Scholar 

  26. Freundlich, A., Bensaoula, A., Bensaoula, A. H. & Rossignol, V. Interface and relaxation properties of chemical beam epitaxy grown GaP/GaAs structures. J. Vac. Sci. Technol. B 11, 843–846 (1993).

    Article  CAS  Google Scholar 

  27. Morales, F. M. et al. Microstructural improvements of InP on GaAs (001) grown by molecular beam epitaxy by in situ hydrogenation and postgrowth annealing. Appl. Phys. Lett. 94, 41919 (2009).

    Article  Google Scholar 

  28. Bae, S.-H. et al. Unveiling the carrier transport mechanism in epitaxial graphene for forming wafer-scale, single-domain graphene. Proc. Natl Acad. Sci. USA 114, 4082–4086 (2017).

    Article  CAS  Google Scholar 

  29. Shim, J. et al. Controlled crack propagation for atomic precision handling of wafer-scale two-dimensional materials. Science 362, 665–670 (2018).

    Article  CAS  Google Scholar 

  30. Kim, J. et al. Layer-resolved graphene transfer via engineered strain layers. Science 342, 833–836 (2013).

    Article  CAS  Google Scholar 

  31. Bae, S.-H. et al. Integration of bulk materials with two-dimensional materials for physical coupling and applications. Nat. Mater. 18, 550–560 (2019).

    Article  CAS  Google Scholar 

  32. Kum, H. et al. Epitaxial growth and layer-transfer techniques for heterogeneous integration of materials for electronic and photonic devices. Nat. Electron. 2, 439–450 (2019).

    Article  CAS  Google Scholar 

  33. Han, Y. et al. Sub-nanometre channels embedded in two-dimensional materials. Nat. Mater. 17, 129–133 (2018).

    Article  CAS  Google Scholar 

  34. Hÿtch, M. J., Snoeck, E. & Kilaas, R. Quantitative measurement of displacement and strain fields from HREM micrographs. Ultramicroscopy 74, 131–146 (1998).

    Article  Google Scholar 

Download references

Acknowledgements

This work is supported by the Defense Advanced Research Projects Agency Young Faculty Award (award no. 029584-00001), the Department of Energy Solar Energy Technologies Office (award no. DE-EE0008558), the Air Force Research Laboratory (award no. FA9453-18-2-0017), ROHM Co., and LG electronics. Y.H. and D.M. were supported by the National Science Foundation Division of Material Research (award no. 1719875). We are grateful for general support from J.S. Lee (Head of the Materials and Devices Advanced Research Institute, LG Electronics).

Author information

Author notes

  1. These authors contributed equally: Sang-Hoon Bae, Kuangye Lu, Yimo Han, Sungkyu Kim.

Authors and Affiliations

  1. Department of Mechanical Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA

    Sang-Hoon Bae, Kuangye Lu, Sungkyu Kim, Kuan Qiao, Hyunseok Kim, Hyun S. Kum, Peng Chen, Wei Kong, Beom-Seok Kang, Chansoo Kim, Jaeyong Lee, Jaewoo Shim & Jeehwan Kim

  2. Research Laboratory of Electronics, Massachusetts Institute of Technology, Cambridge, MA, USA

    Sang-Hoon Bae, Kuangye Lu, Sungkyu Kim, Kuan Qiao, Chanyeol Choi, Hyunseok Kim, Hyun S. Kum, Peng Chen, Wei Kong, Beom-Seok Kang, Chansoo Kim, Jaeyong Lee, Jaewoo Shim & Jeehwan Kim

  3. School of Applied and Engineering Physics, Cornell University, Ithaca, NY, USA

    Yimo Han & David A. Muller

  4. Department of Electrical Engineering and Computer Science, Massachusetts Institute of Technology, Cambridge, MA, USA

    Chanyeol Choi

  5. Materials Science Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA

    Yifan Nie

  6. Electrical and Computer Engineering, Materials Science and Engineering, University of Virginia, Charlottesville, VA, USA

    Yongmin Baek & Kyusang Lee

  7. Materials & Devices Advanced Research Institute, LG Electronics, Seoul, Republic of Korea

    Jinhee Park & Minho Joo

  8. Kavli Institute at Cornell for Nanoscale Science, Cornell University, Ithaca, NY, USA

    David A. Muller

  9. Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA

    Jeehwan Kim

Authors
  1. Sang-Hoon Bae
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Kuangye Lu
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Yimo Han
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Sungkyu Kim
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Kuan Qiao
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Chanyeol Choi
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Yifan Nie
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. Hyunseok Kim
    View author publications

    You can also search for this author in PubMed Google Scholar

  9. Hyun S. Kum
    View author publications

    You can also search for this author in PubMed Google Scholar

  10. Peng Chen
    View author publications

    You can also search for this author in PubMed Google Scholar

  11. Wei Kong
    View author publications

    You can also search for this author in PubMed Google Scholar

  12. Beom-Seok Kang
    View author publications

    You can also search for this author in PubMed Google Scholar

  13. Chansoo Kim
    View author publications

    You can also search for this author in PubMed Google Scholar

  14. Jaeyong Lee
    View author publications

    You can also search for this author in PubMed Google Scholar

  15. Yongmin Baek
    View author publications

    You can also search for this author in PubMed Google Scholar

  16. Jaewoo Shim
    View author publications

    You can also search for this author in PubMed Google Scholar

  17. Jinhee Park
    View author publications

    You can also search for this author in PubMed Google Scholar

  18. Minho Joo
    View author publications

    You can also search for this author in PubMed Google Scholar

  19. David A. Muller
    View author publications

    You can also search for this author in PubMed Google Scholar

  20. Kyusang Lee
    View author publications

    You can also search for this author in PubMed Google Scholar

  21. Jeehwan Kim
    View author publications

    You can also search for this author in PubMed Google Scholar

Contributions

J.K., S.-H.B., K. Lu, Y.H., S.K. and K. Lee conceived the experiment. S.-H.B., K. Lu and H.K. contributed to the epitaxial growth. S.-H.B., K. Lu, B.-S.K., C.K. and J.S. worked on the graphene transfer. Y.H. and S.K. performed the TEM. S.-H.B., K. Lu, Y.H., S.K., D.A.M., K. Lee and J.K. analysed the TEM data. K.Q., W.K. and Y.B. analysed the Raman spectra. C.C. and Y.N. designed and performed the DFT calculation. B.-S.K. and J.L. contributed to the modelling data summary and figure configuration. K. Lu, H.S.K. and P.C. performed XRD. K. Lu and H.K. carried out the EBSD measurement. S.-H.B., K.Q., J.P., M.J. and J.K. contributed to the strain relaxation analysis. All the authors contributed to the discussion and analysis of the results regarding the manuscript. J.K. directed the team.

Corresponding authors

Correspondence to Kyusang Lee or Jeehwan Kim.

Ethics declarations

Competing interests

The authors declare no competing 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 Figs. 1–11, discussion.

Source data

Source Data Fig. 1

Raman data, % relaxation data.

Source Data Fig. 2

Lattice constant of InGaP on bare GaAs substrates along the x-axis and lattice constant of InGaP on graphene-coated GaAs substrates along the y-axis.

Source Data Fig. 3

Energy barrier required for the interface sliding of epilayers on graphene/substrates and bare substrates, threshold energy for each situation and critical thickness of the heteroepitaxy film.

Source Data Fig. 4

HRXRD azimuthal off-axis φ scan of the GaP epilayer.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Bae, SH., Lu, K., Han, Y. et al. Graphene-assisted spontaneous relaxation towards dislocation-free heteroepitaxy. Nat. Nanotechnol. 15, 272–276 (2020). https://doi.org/10.1038/s41565-020-0633-5

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/s41565-020-0633-5

This article is cited by

Search

Advanced 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