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Abstract The improvement of comprehensive properties including hardness, toughness, wear, and corrosion resistance in the transition-metal carbides/nitrides (TMC(N)) films, especially avoiding the trade-off between the hardness and toughness, is strongly required for various applications. Herein, we provide a new strategy, by activating solid-state dewetting during layered deposition, to accomplish the self-assembly of ordered TaC@Ta core–shell-like nanocomposite film consisting of TaC nanocrystallines encapsulated with thin pseudocrystal Ta tissues (∼1.5 nm). The novel core−shell-like structure can simultaneously achieve superhardness (∼45.1 GPa) mainly dominated by the Orowan strengthening mechanism and high toughness attributed to the indenter-induced phase transformation from the pseudocrystal to body-centered cubic α-Ta, together with drastically enhanced wear and corrosion resistance. Furthermore, thin pseudocrystal Ta encapsulated layer (∼1.5 nm) in the TaC@Ta core–shell-like structure helps for promoting the formation of lubricious TaO x Magnéli phase during sliding, thereby further dropping the coefficient of friction relative to TaC monolayer. Apparently, solid-state dewetting may provide a new route to construct ordered TMC(N)@TM core–shell-like nanocomposite structure capable of combining superhardness, high toughness, low friction, and superior wear and corrosion resistance. Graphical abstract Image 1 [ABSTRACT FROM AUTHOR]

Abstract: We have deposited germanium carbide (Ge1−x C x ) films on Si(100) substrate via radio-frequency (RF) reactive magnetron sputtering in a CH4/Ar mixture discharge, and explored the effects of carbon content (x) on the chemical bonding and hardness for the obtained films. We find that x significantly influences the chemical bonding, which leads to a pronounced change in the hardness of the film. To reveal the relationship between the chemical bonding and hardness, first-principles calculations have been carried out. It is shown that as x increases from 0 to 0.33, the fraction of sp3 C–Ge bonds in the film increases at the expense of Ge–Ge bonds, which promotes formation of a strong covalently bonded network, and thus enhances the hardness of the film. However, as x further increases from 0.33 to 0.59, the fraction of sp3 C–Ge bonds in the film gradually reduces, while that of sp3 C–H and graphite-like sp2 C–C bonds increases, which damages the compact network structure, resulting in a sharp decrease in the hardness. This investigation suggests that the medium x (0.17