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Tetrahedral amorphous carbon coatings have the potential to significantly reduce friction and wear between sliding components. Here, we provide atomistic insights into the evolution of the sliding interface between naked and hydrogen-passivated ta-C sliding partners under dry and lubricated conditions. Using reactive classical atomistic simulations we show that sliding induces a sp3 to sp2 rehybridization and that the shear resistance is reduced by hydrogen-passivation and hexadecane-lubricationdespite our finding that nanoscale hexadecane layers are not always able to separate and protect ta-C counter surfaces during sliding. As asperities deform, carbon atoms within the hexadecane lubricant bind to the ta-C sliding partners resulting in degradation of the hexadecane molecules and in increased material intermixing at the sliding interface. Hydrogen atoms from the passivation layer and from the hexadecane chains continue to be mixed within a sp2 rich sliding interface eventually generating a tribo-

Surface passivation and boundary lubrication of self-mated tetrahedral amorphous carbon asperities under extreme tribological conditions