ABSTRACTVapor deposition of smooth, microstructurally uniform amorphous films on dissimilar substrates requires coalescence of clusters that form during initial nucleation. We have developed techniques that provide sub-monolayer sensitivity to this phenomenon, relying on real time spectroscopie ellipsometry observations during ultrathin film growth (thicknesses < 50 Å). An investigation of tetrahedrally-bonded amorphous semiconductors lends insights into the role of nucleation density and adatom surface diffusion in determining the ultimate atomic-scale roughness on the film.