Morphological Evolution of Ag/Mica Films Grown by Pulsed Laser Deposition

Many vapor-deposited metal-on-insulator films exhibit a morphological progression with increasing thickness consisting of several distinct stages: (1) nucleation of 3-dimensional nanocrystalline islands; (2) elongation of the islands; (3) film percolation. Here we report a study of this progression during Pulsed Laser Deposition (PLD), a technique for film deposition that differs from thermal deposition in that the depositing species arrive in short energetic bursts, leading to instantaneous deposition fluxes orders of magnitude higher than can be achieved in thermal growth. Atomic Force Microscopy reveals that advancement through this same morphological progression occurs at lower thickness in PLD films relative to films grown under comparable conditions by thermal deposition, with PLD films having lower RMS roughness at a given thickness. We also observe that for a constant amount deposited per pulse, films deposited at higher laser pulse frequency are further advanced in morphological state. Kinetic Monte Carlo simulations reveal that PLD nucleation behavior differs from that of thermally deposited films, and this can account for the observed differences. Simulations also reveal a scaling of the percolation thickness with pulse frequency that is consistent with experiment.