Nanostructural characterization of amorphous diamondlike carl,on (a-C) film
s grown on silicon using pulsed-laser deposition (PLD) is correlated to bot
h growth energetics and film thickness. Raman spectroscopy and x-ray reflec
tivity probe both the topological nature of three and four-fold coordinated
carbon atom bonding and the topographical clustering of their distribution
s 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 differe
nt for material near the substrate interface compared to material within th
e bulk portion of an a-C film. A simple model balancing the energy of resid
ual stress and the free energies of resulting carbon topologies is proposed
to provide an explanation of the evolution of topographical bonding cluste
rs in a growing a-C film.