Nanostructural characterization of amorphous diamondlike carbon films

Nanostructural characterization of amorphous diamondlike carbon $(a-\mathrm{C})$ films grown on silicon using pulsed-laser deposition (PLD) is correlated to both growth energetics and film thickness. Raman spectroscopy and x-ray reflectivity probe both the topological nature of three- and four-fold coordinated carbon atom bonding and the topographical clustering of their distributions within a given film. In general, increasing the energetics of PLD growth results in films becoming more “diamondlike,” i.e., increasing mass density and decreasing optical absorbance. However, these same properties decrease appreciably with thickness. The topology of carbon atom bonding is different for material near the substrate interface compared to material within the bulk portion of an $a-\mathrm{C}$ film. A simple model balancing the energy of residual stress and the free energies of resulting carbon topologies is proposed to provide an explanation of the evolution of topographical bonding clusters in a growing $a-\mathrm{C}$ film.