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:

The evolving quality of frictional contact with graphene

Nature volume 539, pages 541–545 (2016)Cite this article

Subjects

Abstract

Graphite and other lamellar materials are used as dry lubricants for macroscale metallic sliding components and high-pressure contacts. It has been shown experimentally that monolayer graphene exhibits higher friction than multilayer graphene and graphite, and that this friction increases with continued sliding, but the mechanism behind this remains subject to debate. It has long been conjectured that the true contact area between two rough bodies controls interfacial friction1. The true contact area, defined for example by the number of atoms within the range of interatomic forces, is difficult to visualize directly but characterizes the quantity of contact. However, there is emerging evidence that, for a given pair of materials, the quality of the contact can change, and that this can also strongly affect interfacial friction2,3,4,5,6,7. Recently, it has been found that the frictional behaviour of two-dimensional materials exhibits traits8,9,10,11,12,13 unlike those of conventional bulk materials. This includes the abovementioned finding that for few-layer two-dimensional materials the static friction force gradually strengthens for a few initial atomic periods before reaching a constant value. Such transient behaviour, and the associated enhancement of steady-state friction, diminishes as the number of two-dimensional layers increases, and was observed only when the two-dimensional material was loosely adhering to a substrate8. This layer-dependent transient phenomenon has not been captured by any simulations14,15. Here, using atomistic simulations, we reproduce the experimental observations of layer-dependent friction and transient frictional strengthening on graphene. Atomic force analysis reveals that the evolution of static friction is a manifestation of the natural tendency for thinner and less-constrained graphene to re-adjust its configuration as a direct consequence of its greater flexibility. That is, the tip atoms become more strongly pinned, and show greater synchrony in their stick–slip behaviour. While the quantity of atomic-scale contacts (true contact area) evolves, the quality (in this case, the local pinning state of individual atoms and the overall commensurability) also evolves in frictional sliding on graphene. Moreover, the effects can be tuned by pre-wrinkling. The evolving contact quality is critical for explaining the time-dependent friction of configurationally flexible interfaces.

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

Figure 1: Model setup and frictional behaviour for a Si tip sliding over a graphene/a-Si substrate system at 300 K.
Figure 2: Evolution of the atomic-level forces contributing to friction on a monolayer graphene/a-Si substrate.
Figure 3: Simulations of stick–slip friction on monolayer suspended graphene at 300 K.
Figure 4: Evolution of the atomic-level forces contributing to friction on monolayer suspended graphene.

Similar content being viewed by others

References

  1. Szlufarska, I., Chandross, M. & Carpick, R. W. Recent advances in single-asperity nanotribology. J. Phys. D 41, 123001 (2008)

    Article  ADS  Google Scholar 

  2. Dienwiebel, M. et al. Superlubricity of graphite. Phys. Rev. Lett. 92, 126101 (2004)

    Article  ADS  Google Scholar 

  3. Filippov, A. E., Dienwiebel, M., Frenken, J. W. M., Klafter, J. & Urbakh, M. Torque and twist against superlubricity. Phys. Rev. Lett. 100, 046102 (2008)

    Article  ADS  Google Scholar 

  4. Kim, W. K. & Falk, M. L. Atomic-scale simulations on the sliding of incommensurate surfaces: the breakdown of superlubricity. Phys. Rev. B 80, 235428 (2009)

    Article  ADS  Google Scholar 

  5. van Wijk, M., Dienwiebel, M., Frenken, J. & Fasolino, A. Superlubric to stick-slip sliding of incommensurate graphene flakes on graphite. Phys. Rev. B 88, 235423 (2013)

    Article  ADS  Google Scholar 

  6. Li, Q., Tullis, T. E., Goldsby, D. & Carpick, R. W. Frictional ageing from interfacial bonding and the origins of rate and state friction. Nature 480, 233–236 (2011)

    Article  ADS  CAS  Google Scholar 

  7. Liu, Y. & Szlufarska, I. Chemical origins of frictional aging. Phys. Rev. Lett. 109, 186102 (2012)

    Article  ADS  Google Scholar 

  8. Lee, C. et al. Frictional characteristics of atomically thin sheets. Science 328, 76–80 (2010)

    Article  ADS  CAS  Google Scholar 

  9. Chhowalla, M. & Amaratunga, G. A. Thin films of fullerene-like MoS2 nanoparticles with ultralow friction and wear. Nature 407, 164–167 (2000)

    Article  ADS  CAS  Google Scholar 

  10. Choi, J. S. et al. Friction anisotropy-driven domain imaging on exfoliated monolayer graphene. Science 333, 607–610 (2011)

    Article  ADS  CAS  Google Scholar 

  11. Deng, Z. et al. Nanoscale interfacial friction and adhesion on supported versus suspended monolayer and multilayer graphene. Langmuir 29, 235–243 (2013)

    Article  Google Scholar 

  12. Cho, D.-H. et al. Effect of surface morphology on friction of graphene on various substrates. Nanoscale 5, 3063–3069 (2013)

    Article  ADS  CAS  Google Scholar 

  13. Filleter, T. et al. Friction and dissipation in epitaxial graphene films. Phys. Rev. Lett. 102, 086102 (2009)

    Article  ADS  CAS  Google Scholar 

  14. Ye, Z., Tang, C., Dong, Y. & Martini, A. Role of wrinkle height in friction variation with number of graphene layers. J. Appl. Phys. 112, 116102 (2012)

    Article  ADS  Google Scholar 

  15. Smolyanitsky, A., Killgore, J. & Tewary, V. Effect of elastic deformation on frictional properties of few-layer graphene. Phys. Rev. B 85, 035412 (2012)

    Article  ADS  Google Scholar 

  16. Ishigami, M., Chen, J. H., Cullen, W. G., Fuhrer, M. S. & Williams, E. D. Atomic structure of graphene on SiO2 . Nano Lett. 7, 1643–1648 (2007)

    Article  ADS  CAS  Google Scholar 

  17. Mate, C. M., McClelland, G. M., Erlandsson, R. & Chiang, S. Atomic-scale friction of a tungsten tip on a graphite surface. Phys. Rev. Lett. 59, 1942–1945 (1987)

    Article  ADS  CAS  Google Scholar 

  18. Bonelli, F., Manini, N., Cadelano, E. & Colombo, L. Atomistic simulations of the sliding friction of graphene flakes. Eur. Phys. J. B 70, 449–459 (2009)

    Article  ADS  CAS  Google Scholar 

  19. Li, Q., Lee, C., Carpick, R. W. & Hone, J. Substrate effect on thickness-dependent friction on graphene. Phys. Stat. Sol. B 247, 2909–2914 (2010)

    Article  ADS  CAS  Google Scholar 

  20. Luan, B. & Robbins, M. O. The breakdown of continuum models for mechanical contacts. Nature 435, 929–932 (2005)

    Article  ADS  CAS  Google Scholar 

  21. He, G., Müser, M. H. & Robbins, M. O. Adsorbed layers and the origin of static friction. Science 284, 1650–1652 (1999)

    Article  ADS  CAS  Google Scholar 

  22. Liu, Z. et al. Observation of microscale superlubricity in graphite. Phys. Rev. Lett. 108, 205503 (2012)

    Article  ADS  Google Scholar 

  23. Mohammadi, H. & Müser M. H. Friction of wrinkles. Phys. Rev. Lett. 105, 224301 (2010)

    Article  ADS  Google Scholar 

  24. Spear, J. C., Custer, J. P. & Batteas, J. D. The influence of nanoscale roughness and substrate chemistry on the frictional properties of single and few layer graphene. Nanoscale 7, 10021–10029 (2015)

    Article  ADS  CAS  Google Scholar 

  25. Tersoff, J. Empirical interatomic potential for carbon, with applications to amorphous carbon. Phys. Rev. Lett. 61, 2879–2882 (1988)

    Article  ADS  CAS  Google Scholar 

  26. Stillinger, F. H. & Weber, T. A. Computer simulation of local order in condensed phases of silicon. Phys. Rev. B 31, 5262–5271 (1985)

    Article  ADS  CAS  Google Scholar 

  27. Zacharia, R., Ulbricht, H. & Hertel, T. Interlayer cohesive energy of graphite from thermal desorption of polyaromatic hydrocarbons. Phys. Rev. B 69, 155406 (2004)

    Article  ADS  Google Scholar 

  28. Zong, Z., Chen, C.-L., Dokmeci, M. R. & Wan, K.-t. Direct measurement of graphene adhesion on silicon surface by intercalation of nanoparticles. J. Appl. Phys. 107, 026104 (2010)

    Article  ADS  Google Scholar 

  29. Koenig, S. P., Boddeti, N. G., Dunn, M. L. & Bunch, J. S. Ultrastrong adhesion of graphene membranes. Nat. Nanotechnol. 6, 543–546 (2011)

    Article  ADS  CAS  Google Scholar 

  30. Nosé, S. A unified formulation of the constant temperature molecular-dynamics methods. J. Chem. Phys. 81, 511–519 (1984)

    Article  ADS  Google Scholar 

  31. Plimpton, S. Fast parallel algorithms for short-range molecular dynamics. J. Comput. Phys. 117, 1–19 (1995)

    Article  ADS  CAS  Google Scholar 

  32. Li, J. AtomEye: an efficient atomistic configuration viewer. Model. Simul. Mater. Sci. Eng. 11, 173 (2003)

    Article  ADS  Google Scholar 

  33. Giannazzo, F., Sonde, S., Nigro, R. L., Rimini, E. & Raineri, V. Mapping the density of scattering centers limiting the electron mean free path in graphene. Nano Lett. 11, 4612–4618 (2011)

    Article  ADS  CAS  Google Scholar 

Download references

Acknowledgements

S.L. and P.G. appreciate support from the Alexander von Humboldt Foundation and the Helmholtz Programme Science and Technology of Nanosystems (STN). Q.L., X.D. and J.S. appreciate support from the 973 Programs of China (grant numbers 2013CB933003, 2013CB934201, 2015CB351903 and 2012CB619402), the NSFC (grant numbers 11422218, 11272177, 11432008, 51320105014 and 51321003), the International Joint Laboratory for Micro/Nano Manufacturing and Measurement Technologies, the Tsinghua University Initiative Scientific Research Program (grant number 2014Z01007), the Thousand Young Talents Program of China and 111 project (grant number B06025). R.W.C. acknowledges support from the NSF (grant numbers CMMI-1401164 and MRSEC DMR-1120901). J.L. acknowledges support from the NSF (grant numbers MRSEC DMR-1120901, CBET-1240696, DMR-1410636 and ECCS-1610806). We also thank J. Feng for discussions.

Author information

Authors and Affiliations

  1. State Key Laboratory for Mechanical Behavior of Materials and Frontier Institute of Science and Technology, Xi’an Jiaotong University, Xi’an, 710049, China

    Suzhi Li, Xiangdong Ding, Jun Sun & Ju Li

  2. Department of Nuclear Science and Engineering and Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, 02139, Massachusetts, USA

    Suzhi Li & Ju Li

  3. Institute of Nanotechnology, Karlsruhe Institute of Technology, Eggenstein-Leopoldshafen, 76344, Germany

    Suzhi Li

  4. Center for Nano and Micro Mechanics, Applied Mechanics Laboratory, School of Aerospace Engineering, Tsinghua University, Beijing, 100084, China

    Qunyang Li

  5. State Key Laboratory of Tribology, Tsinghua University, Beijing, 100084, China

    Qunyang Li

  6. Department of Mechanical Engineering and Applied Mechanics, University of Pennsylvania, Philadelphia, 19104, Pennsylvania, USA

    Robert W. Carpick & Xin Z. Liu

  7. Institute for Applied Materials, Karlsruhe Institute of Technology, Karlsruhe, 76131, Germany

    Peter Gumbsch

  8. Fraunhofer Institute for Mechanics of Materials IWM, Freiburg, 79108, Germany

    Peter Gumbsch

  9. Center for Advancing Materials Performance from the Nanoscale (CAMP-Nano), School of Materials Science and Engineering, Xi’an Jiaotong University, Xi’an, 710049, China

    Jun Sun & Ju Li

Authors
  1. Suzhi Li
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Qunyang Li
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Robert W. Carpick
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Peter Gumbsch
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Xin Z. Liu
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Xiangdong Ding
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Jun Sun
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. Ju Li
    View author publications

    You can also search for this author in PubMed Google Scholar

Contributions

Q.L., R.W.C. and J.L. conceived and designed the project. S.L. performed molecular dynamics simulations. Q.L., R.W.C. and X.Z.L. provided information about the atomic force microscope experiments. Q.L., P.G., X.D., J.S. and J.L. provided the simulation guideline. S.L., Q.L., R.W.C. and J.L. wrote the paper. All authors contributed to discussions and analyses of the results.

Corresponding authors

Correspondence to Qunyang Li, Robert W. Carpick or Ju Li.

Ethics declarations

Competing interests

The authors declare no competing financial interests.

Supplementary information

Supplementary Information

This file contains Supplementary Discussions 1-14, Supplementary Figures 1-18, Supplementary Table 1 and Supplementary References. It provides the additional information for the simulation results and relevant discussions. (PDF 7143 kb)

Evolution of graphene configuration during sliding in 1L/a-Si substrate system

This video shows the evolution of graphene configuration of 1L graphene/a-Si substrate in a 2.5nm scan. Colours are shown according to the height amplitude of graphene along the y direction. (MP4 15096 kb)

PowerPoint slides

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Li, S., Li, Q., Carpick, R. et al. The evolving quality of frictional contact with graphene. Nature 539, 541–545 (2016). https://doi.org/10.1038/nature20135

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/nature20135

This article is cited by

Comments

By submitting a comment you agree to abide by our Terms and Community Guidelines. If you find something abusive or that does not comply with our terms or guidelines please flag it as inappropriate.

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