Achieving ultra-hard surface of mechanically polished diamond crystal by thermo-chemical refinement

In the present work, we propose a novel thermo-chemical post-processing method for refining the mechanically polished surface of natural diamond crystal. The deformation mechanisms of diamond crystal during mechanical polishing are elucidated by Raman Spectroscopy corroborated by molecular dynamics simulations. Moreover, the surface mechanical properties of diamond crystal are qualitatively characterized by nanoindentation tests. Our results reveal that under mechanical polishing there are phase transformations from diamond carbons to layered graphite, amorphous sp3 and sp2 hybrided structures occurred in the topmost surface layer, which consequently deteriorates the intrinsic surface strength of diamond crystal. In the following thermo-chemical refinement, the polishing-induced amorphous carbons, layered graphite and internal stress are largely removed through the weak oxidation reaction. It is found that the formation of considerable graphene structures in the topmost surface layer results in an ultra-hard diamond crystal surface with dramatically enhanced hardness and Young's modulus. Our findings shed light on the preparation of natural diamond crystal surface with superior mechanical properties.