Study of thin film growth kinetics of homoepitaxy by molecular beam epitaxy and pulsed laser deposition

This thesis presents an extensive study of the growth kinetics during low temperature homoepitaxy by Molecular Beam Epitaxy (MBE) and Pulsed Laser Deposition (PLD) of our model system Ge(001). The range of the study covers from the sub-monolayer (sub-ML) regime to the later stage where film thickness amounts to a few thousand MLs; it also covers epitaxial breakdown in which epitaxial growth is no longer sustained and the growing phase becomes amorphous. First, we have conducted a systematic investigation of the phase shift of the RHEED intensity oscillations during Ge(001) homoepitaxy MBE for a wide range of diffraction conditions. We conclude that the phase shift is caused by the overlap of the specular spot and the Kikuchi features, in contrast to models involving dynamical scattering theory for the phase shift. We have studied the sub-ML growth of Ge(001) homoepitaxy by MBE at low temperatures using RHEED intensity oscillations obtained for a range of low incidence angles where the influence of the dynamical nature of electron scattering such as the Kikuchi features is minimized. We have developed a new model for RHEED specular intensity that includes the diffuse scattering off surface steps and the layer interference between terraces of different heights using the kinematic approximation. By using the model to interpret the measured RHEED intensity, we find the evolution of the coverage of the first 2-3 layers, from which we infer the ES barrier height to be 0.077 ± 0.014 eV. Finally, using a dual MBE-PLD UHV chamber, we have conducted experiments under identical thermal, background, and surface preparation conditions to compare Ge(001) homoepitaxial growth morphology in PLD and MBE at low temperatures. To isolate the effect of kinetic energy of depositing species during PLD, we varied the average kinetic energy: ∼450 eV in PLD-HKE, ∼300 eV in PLD-LKE, and <1 eV in PLD-TH. At 150°C, we find that in PLD-LKE and in MBE the film morphology evolves in a similar fashion: initially irregularly shaped mounds form, followed by pyramidal mounds with edges of the square-base along <100> directions. The areal feature density is higher for PLD films than for MBE films grown at the same average growth rate and temperature. Furthermore, the dependence upon film thickness of roughness and feature separation differ for PLD and MBE. The thicknesses at which epitaxial breakdown occurs are ranked in the order PLD-HKE > PLD-LKE > MBE. At 100°C, PLD-LKE and MBE follow the same morphology evolution as at 150°C. The epitaxial thicknesses are ranked in the order PLD-LKE > MBE > PLD-TH; additionally, the surface is smoother in PLD-LKE than in MBE. Together, these results convincingly demonstrate that the enhancement of epitaxial growth--the reduction in roughness and the delay of epitaxial breakdown--are due to the kinetic energy of depositing species in PLD. To study the relaxation behavior, we varied the repetition rate from 5 Hz to 20 Hz in PLD-LKE at 100°C. However, we find no systematic effect on surface roughness by varying the repetition rate. This result is consistent with an investigation on the sub-ML growth regime of PLD-LKE by monitoring the intensity variations of the RHEED specular spot.