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Formation and Mechanical Behavior of Nanocomposite Superstructures from Interlayer Bonding in Twisted Bilayer Graphene.

We report a comprehensive study on the design of two-dimensional graphene-diamond nanocomposite superstructures formed through interlayer covalent bonding of twisted bilayer graphene with commensurate bilayers. The interlayer bonding is induced by patterned hydrogenation that leads to the formation of superlattices of two-dimensional nanodiamond domains embedded between the two graphene layers. We generalize a rigorous algorithm for the formation of all possible classes of these superstructures: the structural parameters employed to design such carbon nanocomposites include the commensurate bilayer's twist angle, the stacking type of the nanodomains where the interlayer bonds are formed, the interlayer bond pattern, and the interlayer C-C bond density that is proportional to the concentration of sp3-hybridized interlayer-bonded C atoms. We also analyze systematically the mechanical behavior of these nanocomposite superstructures on the basis of molecular-dynamics simulations of uniaxial tensile straining tests according to a reliable interatomic bond-order potential. We identify a range of structural parameters over which the fracture of these superstructures is ductile, mediated by void formation, growth, and coalescence, contrary to the typical brittle fracture of graphene. We introduce a ductility metric as an order parameter for the brittle-to-ductile transition, demonstrate its direct dependence on the fraction of sp3-hybridized interlayer-bonded C atoms, and show that increasing the fraction of interlayer-bonded C atoms beyond a critical level in certain classes of these superstructures induces their ductile mechanical response.