Ab initio thermodynamics for the growth of ultra-thin Cu film on a perfect MgO(001) surface

Controlled growth of thin metallic films on oxide substrates is important for numerous micro-and nanoelectronic applications. Our ab initio study is devoted to the periodic slab simulations for a series of ordered 2D Cu superlattices on the regular MgO(001) substrate. Submonolayer and monolayer substrate Cu coverages were calculated using the DFT-GGA method, as implemented into the CRYSTAL-98 code. The results of ab initio calculations have been combined with thermodynamic theory which allows us to predict the growth mode of ultra-thin metal films (spinodal decomposition vs. nucleation-and-growth regime) as a function of the metal coverage and the temperature, and to estimate the metal density in clusters. We show that 3D cluster formation becomes predominant already at low Cu coverages, in agreement with the experiment.