| Pulsed laser deposition (PLD) film growth differs from conventional thermal deposition in two essential ways: the depositing species arrive in short bursts of 10--100mus, and with 10--100 eV of kinetic energy. This thesis presents a comprehensive study of the influence of these separate characteristics of the PLD flux on film growth, with the goal of understanding what mechanisms and processes govern PLD morphology evolution.; A theoretical description of the early stages of pulsed, non-energetic growth is presented, with the principal results being a discussion of the dimensionless parameters that must be controlled to achieve data collapse for a variety of conditions; the identification of at least four different island size distribution shapes, which characterize the growth mode being observed; and a rate equation formalism for pulsed deposition that gives excellent agreement with results from kinetic Monte Carlo (KMC) simulations.; The model system of metal-on-insulator film growth has been studied extensively for thermal deposition, and is known to exhibit a characteristic morphological progression beginning with isolated three-dimensional islands and ending with a percolating, continuous film that conducts electrically. Two separate experimental investigations are reported for PLD growth of this system. In the fast, the details of the PLD pulse are held constant and the pulse frequency is varied; this amounts to varying the time-averaged deposition flux. Non-energetic KMC simulations, which take into account only the pulsed nature of the flux, predicted that, for the case where surface diffusion is very fast compared to the pulse frequency and the deposition rate, percolation thickness would scale with pulse frequency with an exponent of -0.34. Experiments performed at 93°C and 135°C gave scaling exponents of -0.31 and -0.34 respectively, in good agreement with the KMC prediction. The experiments also showed good data collapse when maintaining a constant value B/f, where B is the coalescence "efficiency" and f is the pulse frequency.; A separate experimental investigation was performed to compare PLD with thermal deposition under otherwise identical background and substrate conditions; this amounts to studying the effect of varying the average deposition flux. For this case, non-energetic simulations predict that PLD deposits, by virtue of having smaller and more densely spaced islands, would reach percolation with relatively less deposition. (Abstract shortened by UMI.)... |
