Strain shielding from mechanically-activated covalent bond formation in nanoindentation

Abstract

Mechanical failure of an ideal crystal is dictated either by an elastic instability or a soft-mode instability. We show that the ideal strength measurement of graphene based on nano-indentation experiments \cite{lee2008measurement, lee2013high}, however, indicates an anomaly: the inferred strain beneath the diamond indenter at the failure load is anomalously large compared to the fracture strain predicted by soft-mode analysis or acoustic analysis. Here we present a systematic investigation - based on multi-scale modeling combining the results of continuum, atomistic, and quantum calculations; and analysis of experiments - that identifies the operative mechanism responsible for the anomalous difference between the fracture strains. We suggest that a strain-shielding effect due to mechanically-activated covalent bond formation at graphene-indenter interface is responsible for this anomaly. Using Finite Elements Analysis (FEA) and MD simulations of the nanoindentation experiments, we explicitly show that the bonded interaction at the graphene-indenter interface substantially disperses (shields) the strain beneath the indenter, preventing the intensification of strain. Our calculations indicate that the extent of strain shielding depends upon the hydrogen coverage at the indenter surface; and at optimal hydrogen coverage, the strain-shielding effect can delay the onset of fracture to the experimentally-observed indentation load and depth.