ABSTRACTWe apply a rate-equation pair binding model of nucleation kinetics [1] to the nucleation of Si islands grown by hot-wire chemical vapor deposition on SiO2 substrates. Previously, we had demonstrated an increase in grain size of polycrystalline Si films with H2 dilution from 40 nm using 100 mTorr of 1% SiH4 in He to 85 nm with the addition of 20 mTorr H2. [2] This increase in grain size is attributed to atomic H etching of Si monomers rather than stable Si clusters during the early stages of nucleation, decreasing the nucleation density. Atomic force microscopy (AFM) measurements show that the nucleation density increases sublinearly with time at low coverage, implying a fast nucleation rate until a critical density is reached, after which grain growth begins. The nucleation density decreases with increasing H2 dilution (H2:SiH4), which is an effect of the etching mechanism, and with increasing temperature, due to enhanced Si monomer diffusivity on SiO2. From temperature-dependent measurements, we estimate the activation energy for surface diffusion of Si monomers on SiO2 to be 0.47 ± 0.09 eV. Simulations of the temperature-dependent supercritical cluster density lead to an estimated activation energy of 0.42 eV ± 0.01 eV and a surface diffusion coefficient prefactor of 0.1 ± 0.03 cm2/s. H2-dilution-dependent simulations of the supercritical cluster density show an approximately linear relationship between the H2 dilution and the etch rate of clusters.
Accuracy of activation energy from Arrhenius plots and temperature-dependent internal photoemission spectroscopy
