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Graphene nanopattern as a universal epitaxy platform for single-crystal membrane production and defect reduction

Nature Nanotechnology volume 17, pages 1054–1059 (2022)Cite this article

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Abstract

Heterogeneous integration of single-crystal materials offers great opportunities for advanced device platforms and functional systems1. Although substantial efforts have been made to co-integrate active device layers by heteroepitaxy, the mismatch in lattice polarity and lattice constants has been limiting the quality of the grown materials2. Layer transfer methods as an alternative approach, on the other hand, suffer from the limited availability of transferrable materials and transfer-process-related obstacles3. Here, we introduce graphene nanopatterns as an advanced heterointegration platform that allows the creation of a broad spectrum of freestanding single-crystalline membranes with substantially reduced defects, ranging from non-polar materials to polar materials and from low-bandgap to high-bandgap semiconductors. Additionally, we unveil unique mechanisms to substantially reduce crystallographic defects such as misfit dislocations, threading dislocations and antiphase boundaries in lattice- and polarity-mismatched heteroepitaxial systems, owing to the flexibility and chemical inertness of graphene nanopatterns. More importantly, we develop a comprehensive mechanics theory to precisely guide cracks through the graphene layer, and demonstrate the successful exfoliation of any epitaxial overlayers grown on the graphene nanopatterns. Thus, this approach has the potential to revolutionize the heterogeneous integration of dissimilar materials by widening the choice of materials and offering flexibility in designing heterointegrated systems.

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Fig. 1: Graphene nanopattern for single-crystal membrane growth and release.
Fig. 2: APB elimination by graphene nanopatterns.
Fig. 3: Defect reduction in lattice-mismatched heteroepitaxy by graphene nanopatterns.
Fig. 4: Effect of graphene coverage.

Data availability

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

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Acknowledgements

The team at MIT acknowledges support by the Defense Advanced Research Projects Agency Young Faculty Award (award no. 029584-00001), the Air Force Research Laboratory (award no. FA9453-18-2-0017 and FA9453-21-C-0717), the US Department of Energy’s Office of Energy Efficiency and Renewable Energy (EERE) under the Solar Energy Technologies Office (award no. DE-EE0008558), Universiti Tenaga Nasional and UNTEN R&D Sdn. Bhd., Malaysia through TNB Seed fund grant no. U-TV-RD-20-10, and Umicore. STEM was performed at the Center for Electron Microscopy and Analysis (CEMAS) at The Ohio State University. M.Z. and J.H. acknowledge support by the National Science Foundation under NSF award no. DMR-2011876.

Author information

Author notes

  1. These authors contributed equally: Hyunseok Kim, Sangho Lee, Jiho Shin.

Authors and Affiliations

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

    Hyunseok Kim, Sangho Lee, Jiho Shin, Kuangye Lu, Ne Myo Han, Celesta S. Chang, Jun Min Suh, Ki Seok Kim, Bo-In Park, He Yu, Seungju Seo & Jeehwan Kim

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

    Hyunseok Kim, Sangho Lee, Jiho Shin, Kuangye Lu, Ne Myo Han, Celesta S. Chang, Jun Min Suh, Bo-In Park, He Yu, Seungju Seo & Jeehwan Kim

  3. Department of Materials Science and Engineering, The Ohio State University, Columbus, OH, USA

    Menglin Zhu & Jinwoo Hwang

  4. Department of Physics, Applied Physics, and Astronomy, Rensselaer Polytechnic Institute, Troy, NY, USA

    Marx Akl

  5. Department of Electrical and Computer Engineering, University of Virginia, Charlottesville, VA, USA

    Yongmin Baek & Kyusang Lee

  6. Department of Materials Science and Engineering, Rensselaer Polytechnic Institute, Troy, NY, USA

    Yanming Zhang & Yunfeng Shi

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

    Chanyeol Choi

  8. School of Electrical and Electronic Engineering, Yonsei University, Seoul, Republic of Korea

    Heechang Shin, Hyun S. Kum & Jong-Hyun Ahn

  9. Department of Mechanical Engineering and Materials Science, Washington University in Saint Louis, St. Louis, MO, USA

    Yuan Meng & Sang-Hoon Bae

  10. Department of Energy Systems Research and Department of Materials Science and Engineering, Ajou University, Suwon, Republic of Korea

    Seung-Il Kim & Jae-Hyun Lee

  11. Institute of Materials Science and Engineering, Washington University in Saint Louis, St. Louis, MO, USA

    Sang-Hoon Bae

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

    Jeehwan Kim

Authors
  1. Hyunseok Kim
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Contributions

J.K. and S.-H.B. conceived the idea. H.K., S.L. and J.S. designed and coordinated the experiments. M.A., Y.Z. and Y.S. conducted the theoretical studies and simulations of epitaxy. Epitaxial growth was performed by H.K., K. Lu and Y.B. Graphene growth and transfer were performed by H.K., S.L., K. Lu, N.M.H., K.S.K., H.S., H.S.K., S.-I.K., J.-H.L. and J.-H.A. Patterning, exfoliation and device fabrication were performed by S.L., J.S., H.K., K. Lu, B.-I.P., C.C., H.Y., Y.M. and S.S. Exfoliation theory is developed by H.K., S.L., N.M.H., K. Lee, S.-H.B. and J.K. STEM measurements and GPA analysis were conducted by M.Z. and J.H. Material characterizations were conducted by H.K., S.L., N.M.H., K. Lu, C.S.C., J.M.S., H.Y., Y.M. and S.S. Optoelectronic characterizations were conducted by H.K. and J.S. The manuscript was written by H.K., Y.S. and J.K. with input from all the authors. All the authors contributed to the analysis and discussion of the results leading to the manuscript.

Corresponding authors

Correspondence to Sang-Hoon Bae, Jinwoo Hwang, Yunfeng Shi or Jeehwan Kim.

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Supplementary Information

Supplementary Sections 1 and 2 and Figs. 1–23.

Supplementary Video 1

Video of Fig. 3a.

Supplementary Video 2

Video of Fig. 3b.

Supplementary Video 3

Video of Fig. 3c.

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Kim, H., Lee, S., Shin, J. et al. Graphene nanopattern as a universal epitaxy platform for single-crystal membrane production and defect reduction. Nat. Nanotechnol. 17, 1054–1059 (2022). https://doi.org/10.1038/s41565-022-01200-6

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