The evolution of surface roughness on hydrogenated amorphous silicon (a-Si:H) films prepared by plasma-enhanced chemical vapor deposition exhibits initial smoothening due to nuclei coalescence, a region of surface stability, and finally a prominent roughening transition (designated a→a) at a critical thickness. The thickness at which the a→a transition occurs, as measured by real time spectroscopic ellipsometry (SE), is found to correlate closely with the electronic properties of the film. Thus, the transition has been incorporated into deposition phase diagrams that have been applied successfully to optimize solar cell performance and stability. A simple continuum model for the evolution of the 1D surface profile using an initial condition designed to be consistent with the nucleation characteristics measured by real time SE is sufficient for insights into the correlation between the roughness evolution and film properties. Good agreement between the experimental results and model calculations support the concept that optimum electronic properties of the films are associated with weakly reactive surfaces and long lifetime radicals that lead to adsorbed precursors with large surface diffusion lengths.