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Molecular Dynamics Examination of Sliding History-Dependent Adhesion in Si–Si Nanocontacts: Connecting Friction, Wear, Bond Formation, and Interfacial Adhesion

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Abstract

We simulate the contact between nanoscale hydrogen-terminated, single-crystal silicon asperities and surfaces using reactive molecular dynamics (MD) simulations. The results are consistent with recent experimental observations of a more than order-of-magnitude sliding-induced increase in interfacial adhesion for silicon-silicon nanocontact experiments obtained using in situ transmission electron microscopy (TEM). In particular, the MD simulations support the hypothesis that the increased adhesion results from sliding-induced removal of passivating species, in this case hydrogen, followed by rapid formation of Si–Si covalent bonds across the interface, with little plastic deformation of the asperities. The MD results concur with the additional hypothesis that subsequent readsorption of passivating species explains the experimental observation that adhesion reverts to low values upon subsequent contact. However, the simulations further reveal that the sliding-induced adhesion increase is only observed when there are a sufficient number of preexisting surface defects in the form of incomplete hydrogen coverage. Increased hydrogen coverage suppresses interfacial bonding, within the time span of the simulations. Furthermore, the relative alignment of the surface crystal axes plays a strong role in affecting the probability of bond formation during sliding and the subsequent adhesive pull-off force. Also, the hydrogen coverage and sliding distance significantly impact friction at low to moderate hydrogen coverages. Atomic-scale wear does occur during the sliding process primarily through Si–Si bond formation across the interface followed by pull-out of Si atoms from the tip. At low hydrogen coverages, wear is far more severe, Archard’s wear law is obeyed, and significant morphological changes of the asperity occur. The bond formation process is highly stochastic, but shows a general trend of greater numbers of bonds with greater sliding distances. Tips wear by losing large clusters of material, then smaller clusters and individual atoms, and eventually enter into a wearless regime as hydrogen termination increases.

Graphical Abstract

A hydrogen-terminated Si tip (green and blue) in sliding contact with a hydrogen-terminated Si substrate (yellow and red). The sliding direction is indicated by the black arrow. At this level of hydrogen termination, wear is initiated by the removal of hydrogen atoms from the tip (blue atoms at left of figure). Continued sliding causes the formation of interfacial Si-Si bonds followed by the transfer of Si and H from the tip to the surface.

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Acknowledgements

The authors would like to acknowledge Prof. Mark O. Robbins for his ground-breaking contributions to the field of tribology, his mentorship, and the many wonderful discussions the authors have had with Prof. Robbins over the past 25 years. He was generous with his time, kind in spirit, and his absence will be felt by all in the field and most acutely by the authors. While Prof. Robbins is no longer with us, wherever he may be, we wish him fair winds and following seas in the journey. ZM would like to thank Dr. R. Bernal and Dr. H.J. Farnsworth for insightful conversations. RWC, ZM, and JDS acknowledge support from AFOSR/AOARD through Award No. FA2386–18–1-4083.

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Authors and Affiliations

  1. Mechanical Engineering Department, North Carolina A&T University, Greensboro, NC, 27411, USA

    J. David Schall

  2. Nanostructure Physics, Sandia National Laboratories, Albuquerque, NM, 87123, USA

    Zachary B. Milne

  3. Department of Mechanical Engineering and Applied Mechanics, University of Pennsylvania, Philadelphia, PA, USA

    Robert W. Carpick

  4. Chemistry Department, United States Naval Academy, Annapolis, MD, 21402, USA

    Judith A. Harrison

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Schall, J.D., Milne, Z.B., Carpick, R.W. et al. Molecular Dynamics Examination of Sliding History-Dependent Adhesion in Si–Si Nanocontacts: Connecting Friction, Wear, Bond Formation, and Interfacial Adhesion. Tribol Lett 69, 52 (2021). https://doi.org/10.1007/s11249-021-01431-z

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