A two-step Monte Carlo method for atomistically simulating low energy physical vapor deposition processes is developed and used to model the two-dimensional physical vapor deposition of nickel. The method consists of an impact approximation for the initial adatom adsorption on a surface and a multipath diffusion analysis to simulate subsequent surface morphology and interior atomic structure evolution. An embedded atom method is used to determine the activation energies for each of the many available diffusional paths. The method has been used to predict the morphology/structure evolution of nickel films over the length and time scales encountered in practical deposition processes. The modeling approach has enabled determination of the effect of vapor processing variables such as flux orientation, deposition rate and substrate temperature on deposit morphology/ microstructure as defined by packing density, surface roughness and growth column width (which appears closely related to grain size). Several aspects of the empirical Movchan-Demchishin structure zone model are well predicted by this approach.