The two main techniques used to record the data in this dissertation were Spot Profile Analysis - Low Energy Electron Diffraction (SPA-LEED) and Scanning Tunneling Microscopy (STM). A specific data analysis technique for LEED data called G(S) curves is described in depth. G(S) curves can provide a great deal of structural information about the surface; including step heights, island size, and island separation. The effects of quantum size effects (QSE) on the diffusion and critical island sizes of Pb and In on Pb #12;films are reported. Pb depositions on the 2D In phases {radical}3 and {radical}31 to see how the phases affect the Pb growth and its strong QSE are reported.