Why is Superlubricity of Diamond‐Like Carbon Rare at Nanoscale?

Abstract Hydrogenated diamond‐like carbon (HDLC) is a promising solid lubricant for its superlubricity which can benefit various industrial applications. While HDLC exhibits notable friction reduction in macroscale tests in inert or reducing environmental conditions, ultralow friction is rarely observed at the nanoscale. This study investigates this rather peculiar dependence of HDLC superlubricity on the contact scale. To attain superlubricity, HDLC requires i) removal of ≈2 nm‐thick air‐oxidized surface layer and ii) shear‐induced transformation of amorphous carbon to highly graphitic and hydrogenated structure. The nanoscale wear depth exceeds the typical thickness of the air‐oxidized layer, ruling out the possibility of incomplete removal of the air‐oxidized layer. Raman analysis of transfer films indicates that shear‐induced graphitization readily occurs at shear stresses lower than or comparable to those in the nanoscale test. Thus, the same is expected to occur at the nanoscale test. However, the graphitic transfer films are not detected in ex‐situ analyses after nanoscale friction tests, indicating that the graphitic transfer films are pushed out of the nanoscale contact area due to the instability of transfer films within a small contact area. Combining all these observations, this study concludes the retention of highly graphitic transfer films is crucial to achieving HDLC superlubricity.