“…Previous attempts at SE characterization of bulk nanocrystalline and microcrystalline diamond films have predominantly focused on the use of a Bruggeman effective medium approximation (EMA) to mix reference optical indices of the expected constituents and represent the film by a single homogenous medium, − successfully showing incremental improvements in fit upon the addition of components to represent grain boundary sp 2 carbon and void content between the nuclei, and surface roughness. ,,− Although “seed” layers of 15–41 nm adjacent to the substrate rich in sp 2 , void, and occasionally SiC content have been observed with such an approach, ,, parameter correlation with the impurity fractions within the bulk prevents determination of the microstructure of this layer with any confidence . More comprehensively, in situ characterization of the initial stages of diamond growth atop diamond grit-abraded silicon substrates modeled the transition from isolated islands to coalesced film. ,− During these studies, the authors noted an initial parabolic reduction in the void content, indicative of lateral VW-type growth, followed by coalescence and a sharp peak in the sp 2 fraction indicative of the trapping of nondiamond material within the grain boundaries, , accentuated by the large surface/volume ratio of crystallites.…”