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:

Van der Waals device integration beyond the limits of van der Waals forces using adhesive matrix transfer

Nature Electronics volume 7, pages 17–28 (2024)Cite this article

Subjects

Abstract

Pristine van der Waals (vdW) heterostructures formed between two-dimensional (2D) and other materials can be used to create optical and electronic devices. However, the weak vdW forces alone do not allow direct physical stacking of arbitrary layers. As a result, vdW heterostructure fabrication typically requires solvents, sacrificial layers or high temperatures, which can introduce damage and contaminants. Here, we show that adhesive matrix transfer can eliminate these limitations and can provide vdW integration beyond the limits of vdW forces. In the approach, a hybrid high- and low-adhesion surface is used to decouple the forces driving the transfer from the vdW forces defining the heterostructure of interest. We show that the technique can be used to achieve direct vdW integration of diverse 2D materials (MoS2, WSe2, PtS2 and GaS) with dielectrics (SiO2 and Al2O3), which is conventionally forbidden but critical for active devices and scalable, aligned heterostructure formation. The approach also allows single-step 2D material-to-device integration, which we illustrate by fabricating arrays of monolayer MoS2 transistors. As any exposure to solvents or polymers is avoided, the interfaces and surfaces remain pristine. Thus, intrinsic 2D material properties can be probed without the influence of processing steps. The materials can be further engineered through surface treatments and used to fabricate unconventional device form factors.

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: Adhesive matrix transfer of pristine 2D materials.
Fig. 2: Adhesive matrix engineering.
Fig. 3: Polymers as adhesive matrices.
Fig. 4: Patterned, aligned fabrication of vdW heterostructures.
Fig. 5: Single-step adhesive matrix fabrication of pristine MoS2 transistors.

Similar content being viewed by others

Data availability

The data that support the plots within this paper and other findings of this study are available from the corresponding authors on reasonable request.

Code availability

The source code for processing the data is available from the corresponding author upon request.

References

  1. Bhimanapati, G. R. et al. Recent advances in two-dimensional materials beyond graphene. ACS Nano 9, 11509–11539 (2015).

    Article  Google Scholar 

  2. Jariwala, D., Marks, T. J. & Hersam, M. C. Mixed-dimensional van der Waals heterostructures. Nat. Mater. 16, 170–181 (2017).

    Article  Google Scholar 

  3. Liu, Y., Huang, Y. & Duan, X. Van der Waals integration before and beyond two-dimensional materials. Nature 567, 323–333 (2019).

    Article  Google Scholar 

  4. Israelachvili, J. Intermolecular and Surface Forces (Academic Press, 2011).

  5. Schranghamer, T. F., Sharma, M., Singh, R. & Das, S. Review and comparison of layer transfer methods for two-dimensional materials for emerging applications. Chem. Soc. Rev. 50, 11032–11054 (2021).

    Article  Google Scholar 

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

    Article  Google Scholar 

  7. Liang, X. et al. Toward clean and crackless transfer of graphene. ACS Nano 5, 9144–9153 (2011).

    Article  Google Scholar 

  8. Lin, Y.-C. et al. Graphene annealing: how clean can it be? Nano Lett. 12, 414–419 (2012).

    Article  Google Scholar 

  9. Pirkle, A. et al. The effect of chemical residues on the physical and electrical properties of chemical vapor deposited graphene transferred to SiO2. Appl. Phys. Lett. 99, 122108 (2011).

    Article  Google Scholar 

  10. Islam, A., Lee, J. & Feng, P. X. L. All-dry transferred single- and few-layer MoS2 field effect transistor with enhanced performance by thermal annealing. J. Appl. Phys. 123, 025701 (2018).

    Article  Google Scholar 

  11. Castellanos-Gomez, A. et al. Deterministic transfer of two-dimensional materials by all-dry viscoelastic stamping. 2D Mater. 1, 011002 (2014).

    Article  Google Scholar 

  12. Caldwell, J. D. et al. Technique for the dry transfer of epitaxial graphene onto arbitrary substrates. ACS Nano 4, 1108–1114 (2010).

    Article  Google Scholar 

  13. Pizzocchero, F. et al. The hot pick-up technique for batch assembly of van der Waals heterostructures. Nat. Commun. 7, 11894 (2016).

    Article  Google Scholar 

  14. Watson, A. J., Lu, W., Guimarães, M. H. D. & Stöhr, M. Transfer of large-scale two-dimensional semiconductors: challenges and developments. 2D Mater. 8, 032001 (2021).

    Article  Google Scholar 

  15. Liu, Y. et al. Approaching the Schottky–Mott limit in van der Waals metal–semiconductor junctions. Nature 557, 696–700 (2018).

    Article  Google Scholar 

  16. Jung, Y. et al. Transferred via contacts as a platform for ideal two-dimensional transistors. Nat. Electron. 2, 187–194 (2019).

    Article  Google Scholar 

  17. Liu, L. et al. Transferred van der Waals metal electrodes for sub-1-nm MoS2 vertical transistors. Nat. Electron. 4, 342–347 (2021).

    Article  Google Scholar 

  18. Liu, G. et al. Graphene-assisted metal transfer printing for wafer-scale integration of metal electrodes and two-dimensional materials. Nat. Electron. 5, 275–280 (2022).

    Article  Google Scholar 

  19. Poddar, P. K. et al. Resist-free lithography for monolayer transition metal dichalcogenides. Nano Lett. 22, 726–732 (2022).

    Article  Google Scholar 

  20. Velický, M. et al. Strain and charge doping fingerprints of the strong interaction between monolayer MoS2 and gold. J. Phys. Chem. Lett. 11, 6112–6118 (2020).

    Article  Google Scholar 

  21. Liu, F. et al. Disassembling 2D van der Waals crystals into macroscopic monolayers and reassembling into artificial lattices. Science 367, 903–906 (2020).

    Article  Google Scholar 

  22. Heyl, M. et al. Thermally activated gold‐mediated transition metal dichalcogenide exfoliation and a unique gold‐mediated transfer. Phys. Status Solidi Rapid Res. Lett. 14, 2000408 (2020).

    Article  Google Scholar 

  23. Li, Z. et al. Dry exfoliation of large-area 2D monolayer and heterostructure arrays. ACS Nano 15, 13839–13846 (2021).

    Article  MathSciNet  Google Scholar 

  24. Lee, C. et al. Anomalous lattice vibrations of single- and few-layer MoS2. ACS Nano 4, 2695–2700 (2010).

    Article  Google Scholar 

  25. Splendiani, A. et al. Emerging photoluminescence in monolayer MoS2. Nano Lett. 10, 1271–1275 (2010).

    Article  Google Scholar 

  26. Zhao, W. et al. Lattice dynamics in mono- and few-layer sheets of WS2 and WSe2. Nanoscale 5, 9677–9683 (2013).

    Article  Google Scholar 

  27. Zhao, Y. et al. Extraordinarily strong interlayer interaction in 2D layered PtS2. Adv. Mater. 28, 2399–2407 (2016).

    Article  Google Scholar 

  28. Gutiérrez, Y., Giangregorio, M. M., Dicorato, S., Palumbo, F. & Losurdo, M. Exploring the thickness-dependence of the properties of layered gallium sulfide. Front. Chem. 9, 781467 (2021).

    Article  Google Scholar 

  29. Vogel, N., Zieleniecki, J. & Köper, I. As flat as it gets: ultrasmooth surfaces from template-stripping procedures. Nanoscale 4, 3820–3832 (2012).

    Article  Google Scholar 

  30. Velický, M. et al. Mechanism of gold-assisted exfoliation of centimeter-sized transition-metal dichalcogenide monolayers. ACS Nano 12, 10463–10472 (2018).

    Article  Google Scholar 

  31. Bordag, M., Mohideen, U. & Mostepanenko, V. M. New developments in the Casimir effect. Phys. Rep. 353, 1–205 (2001).

    Article  MathSciNet  Google Scholar 

  32. Huang, Y. et al. Universal mechanical exfoliation of large-area 2D crystals. Nat. Commun. 11, 2453 (2020).

    Article  Google Scholar 

  33. Lifshitz, E. M. & Hamermesh, M. The theory of molecular attractive forces between solids. Perspect. Theor. Phys. 26, 329–349 (1992).

    Article  Google Scholar 

  34. Drosdoff, D. & Woods, L. M. Casimir forces and graphene sheets. Phys. Rev. B Condens. Matter Mater. Phys. 82, 155459 (2010).

    Article  Google Scholar 

  35. Khurgin, J. B. Expanding the photonic palette: exploring high index materials. ACS Photonics 9, 743–751 (2022).

    Article  Google Scholar 

  36. Wei, Z. et al. Scratching lithography for wafer-scale MoS2 monolayers. 2D Mater. 7, 045028 (2020).

    Article  Google Scholar 

  37. Liu, X., Howell, S. T., Conde‐Rubio, A., Boero, G. & Brugger, J. Thermomechanical nanocutting of 2D materials. Adv. Mater. 32, 2001232 (2020).

    Article  Google Scholar 

  38. Blake, P. et al. Making graphene visible. Appl. Phys. Lett. 91, 063124 (2007).

    Article  Google Scholar 

  39. Ferrari, A. C. et al. Raman spectrum of graphene and graphene layers. Phys. Rev. Lett. 97, 187401 (2006).

    Article  Google Scholar 

  40. Neumann, C. et al. Raman spectroscopy as probe of nanometre-scale strain variations in graphene. Nat. Commun. 6, 8429 (2015).

    Article  Google Scholar 

  41. Ding, F. et al. Stretchable graphene: a close look at fundamental parameters through biaxial straining. Nano Lett. 10, 3453–3458 (2010).

    Article  Google Scholar 

  42. Lee, J. E., Ahn, G., Shim, J., Lee, Y. S. & Ryu, S. Optical separation of mechanical strain from charge doping in graphene. Nat. Commun. 3, 1024 (2012).

    Article  Google Scholar 

  43. Bendiab, N. et al. Unravelling external perturbation effects on the optical phonon response of graphene. J. Raman Spectrosc. 49, 130–145 (2018).

    Article  Google Scholar 

  44. Aitken, Z. H. & Huang, R. Effects of mismatch strain and substrate surface corrugation on morphology of supported monolayer graphene. J. Appl. Phys. 107, 123531 (2010).

    Article  Google Scholar 

  45. Liu, F., Navaraj, W. T., Yogeswaran, N., Gregory, D. H. & Dahiya, R. Van der Waals contact engineering of graphene field-effect transistors for large-area flexible electronics. ACS Nano 13, 3257–3268 (2019).

    Article  Google Scholar 

  46. Fan, X. et al. Graphene ribbons with suspended masses as transducers in ultra-small nanoelectromechanical accelerometers. Nat. Electron. 2, 394–404 (2019).

    Article  Google Scholar 

  47. Fan, X. et al. Suspended graphene membranes with attached silicon proof masses as piezoresistive nanoelectromechanical systems accelerometers. Nano Lett. 19, 6788–6799 (2019).

    Article  Google Scholar 

  48. Ruiz-Vargas, C. S. et al. Softened elastic response and unzipping in chemical vapor deposition graphene membranes. Nano Lett. 11, 2259–2263 (2011).

    Article  Google Scholar 

  49. Cartamil-Bueno, S. J. et al. Very large scale characterization of graphene mechanical devices using a colorimetry technique. Nanoscale 9, 7559–7564 (2017).

    Article  Google Scholar 

  50. Liu, X., Yuan, Y., Qu, D. & Sun, J. Ambipolar MoS2 field‐effect transistor by spatially controlled chemical doping. Phys. Status Solidi Rapid Res. Lett. 13, 1900208 (2019).

    Article  Google Scholar 

  51. Wang, Y. et al. P-type electrical contacts for 2D transition-metal dichalcogenides. Nature 610, 61–66 (2022).

    Article  Google Scholar 

  52. Pu, J. et al. Highly flexible MoS2 thin-film transistors with ion gel dielectrics. Nano Lett. 12, 4013–4017 (2012).

    Article  Google Scholar 

  53. Cheng, R. et al. Few-layer molybdenum disulfide transistors and circuits for high-speed flexible electronics. Nat. Commun. 5, 5143 (2014).

    Article  Google Scholar 

  54. Daus, A. et al. High-performance flexible nanoscale transistors based on transition metal dichalcogenides. Nat. Electron. 4, 495–501 (2021).

    Article  Google Scholar 

  55. Vogel, N. et al. Laterally patterned ultraflat surfaces. Small 5, 821–825 (2009).

    Article  Google Scholar 

  56. Leplan, H., Geenen, B., Robic, J. Y. & Pauleau, Y. Residual stresses in evaporated silicon dioxide thin films: correlation with deposition parameters and aging behavior. J. Appl. Phys. 78, 962–968 (1995).

    Article  Google Scholar 

  57. Gruber, W. et al. Strain relaxation and vacancy creation in thin platinum films. Phys. Rev. Lett. 107, 265501 (2011).

    Article  Google Scholar 

  58. Soled, S., Wold, A. & Gorochov, O. Crystal growth and characterization of several platinum sulfoselenides. Mater. Res. Bull. 11, 927–932 (1976).

    Article  Google Scholar 

  59. Lieth, R. M. A., Van Der Heijden, C. W. M. & Van Kessel, J. W. M. Preparation, purity and electrical conductivity of gallium sulphide single crystals. J. Cryst. Growth 5, 251–258 (1969).

    Article  Google Scholar 

  60. Li, X. et al. Transfer of large-area graphene films for high-performance transparent conductive electrodes. Nano Lett. 9, 4359–4363 (2009).

    Article  Google Scholar 

  61. Park, H. et al. Optimized poly(methyl methacrylate)-mediated graphene-transfer process for fabrication of high-quality graphene layer. Nanotechnology 29, 415303 (2018).

    Article  Google Scholar 

  62. Her, M., Beams, R. & Novotny, L. Graphene transfer with reduced residue. Phys. Lett. A 377, 1455–1458 (2013).

    Article  Google Scholar 

  63. Ling, X. et al. Role of the seeding promoter in MoS2 growth by chemical vapor deposition. Nano Lett. 14, 464–472 (2014).

    Article  Google Scholar 

  64. Ylivaara, O. M. E. et al. Aluminum oxide from trimethylaluminum and water by atomic layer deposition: the temperature dependence of residual stress, elastic modulus, hardness and adhesion. Thin Solid Films 552, 124–135 (2014).

    Article  Google Scholar 

  65. Li, N. et al. Large-scale flexible and transparent electronics based on monolayer molybdenum disulfide field-effect transistors. Nat. Electron. 3, 711–717 (2020).

    Article  Google Scholar 

Download references

Acknowledgements

This work was supported by the National Science Foundation (NSF; Award No. CMMI-2135846) and the NSF Center for Energy Efficient Electronics Science (Award No. ECCS-0939514). P.F.S., P.J.-P. and S.O.S. acknowledge support from the NSF Graduate Research Fellowship Program (Grant No. 1745302). The work by H.G. and X.L. was supported by the US Department of Energy, Office of Science, Basic Energy Sciences (Award No. DE-SC0021064). The work by X.L., Q.T. and H.K. was supported by the NSF (Award No. CHE-1945364). H.G. acknowledges support from a BUnano Cross-Disciplinary Fellowship at Boston University. A.-Y.L. and J.K. acknowledge support from the US Army Research Office through the Institute for Soldier Nanotechnologies at the Massachusetts Institute of Technology (MIT; Cooperative Agreement No. W911NF-18-2-0048). The fabrication and characterization procedures in this work were in part carried out using the MIT.nano shared facilities. We thank the research staff of MIT.nano, in particular K. Broderick, W. Hess, J. Scholvin, D. Terry and D. Ward, for their support of this work. P.F.S. would further like to thank J. Zhu for electrical measurement advice, N. Romeo for help with mechanical modelling and M. Saravanapavanantham for characterization support. The TEM sample preparation and imaging were performed at the Harvard University Center for Nanoscale Systems with the help of S. Kraemer and J. Gardener. The Center for Nanoscale Systems is a member of the National Nanotechnology Coordinated Infrastructure Network, which is supported by the NSF (ECCS Award No. 1541959).

Author information

Authors and Affiliations

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

    Peter F. Satterthwaite, Patricia Jastrzebska-Perfect, Sarah O. Spector, Ang-Yu Lu, Shin-Yi Tang, Jing Kong & Farnaz Niroui

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

    Peter F. Satterthwaite, Weikun Zhu, Patricia Jastrzebska-Perfect, Sarah O. Spector, Ang-Yu Lu, Jing Kong & Farnaz Niroui

  3. Department of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA

    Weikun Zhu

  4. Department of Physics, Massachusetts Institute of Technology, Cambridge, MA, USA

    Melbourne Tang

  5. Department of Chemistry, Boston University, Boston, MA, USA

    Hongze Gao, Hikari Kitadai, Qishuo Tan & Xi Ling

  6. Department of Materials Science and Engineering, National Tsing Hua University, Hsinchu, Taiwan

    Shin-Yi Tang & Yu-Lun Chueh

  7. Semiconductor Research Center, Hon Hai Research Institute, Taipei, Taiwan

    Shin-Yi Tang

  8. College of Semiconductor Research, National Tsing Hua University, Hsinchu, Taiwan

    Yu-Lun Chueh

  9. Department of Physics, National Cheng Kung University, Tainan, Taiwan

    Chia-Nung Kuo & Chin Shan Lue

  10. Taiwan Consortium of Emergent Crystalline Materials, National Science and Technology Council, Taipei, Taiwan

    Chia-Nung Kuo & Chin Shan Lue

  11. Program on Key Materials, Academy of Innovative Semiconductor and Sustainable Manufacturing, National Cheng Kung University, Tainan, Taiwan

    Chin Shan Lue

  12. Division of Materials Science and Engineering, Boston University, Boston, MA, USA

    Xi Ling

  13. The Photonics Center, Boston University, Boston, MA, USA

    Xi Ling

Authors
  1. Peter F. Satterthwaite
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Weikun Zhu
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Patricia Jastrzebska-Perfect
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Melbourne Tang
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Sarah O. Spector
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Hongze Gao
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Hikari Kitadai
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. Ang-Yu Lu
    View author publications

    You can also search for this author in PubMed Google Scholar

  9. Qishuo Tan
    View author publications

    You can also search for this author in PubMed Google Scholar

  10. Shin-Yi Tang
    View author publications

    You can also search for this author in PubMed Google Scholar

  11. Yu-Lun Chueh
    View author publications

    You can also search for this author in PubMed Google Scholar

  12. Chia-Nung Kuo
    View author publications

    You can also search for this author in PubMed Google Scholar

  13. Chin Shan Lue
    View author publications

    You can also search for this author in PubMed Google Scholar

  14. Jing Kong
    View author publications

    You can also search for this author in PubMed Google Scholar

  15. Xi Ling
    View author publications

    You can also search for this author in PubMed Google Scholar

  16. Farnaz Niroui
    View author publications

    You can also search for this author in PubMed Google Scholar

Contributions

P.F.S. and F.N. conceived the project, designed the experiments and wrote the manuscript. P.F.S. performed the experiments and analysed the results. P.F.S., P.-J.P., W.Z. and F.N. developed the template-stripping process. W.Z. assisted with the photoluminescence measurements. P.F.S., M.T. and F.N. developed the MoS2 transfer process. S.O.S. assisted with TEM sample preparation and imaging. H.G. and X.L. grew the CVD MoS2. S.-Y.T., Y.-L.C., C.-N.K. and C.S.L. grew the PtS2. Q.T. and X.L. grew the GaS. P.F.S., H.K., A.-Y.L., J.K., X.L. and F.N. developed the graphene transfer process. F.N. supervised the project. All authors contributed to finalizing the manuscript.

Corresponding author

Correspondence to Farnaz Niroui.

Ethics declarations

Competing interests

The authors declare no competing interests.

Peer review

Peer review information

Nature Electronics thanks Mengjian Zhu and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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. 1–15, Tables 1–5 and Notes 1–6.

Rights and permissions

Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Satterthwaite, P.F., Zhu, W., Jastrzebska-Perfect, P. et al. Van der Waals device integration beyond the limits of van der Waals forces using adhesive matrix transfer. Nat Electron 7, 17–28 (2024). https://doi.org/10.1038/s41928-023-01079-8

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/s41928-023-01079-8

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