Vapour Phase Synthesis of Thin Films: Towards a Unified Atomistic and Kinetic Framework

The essence of an atomistic unified kinetic model of strained thin film growth and defect initiation is presented along with a comparison of its consequences obtained from computer simulations with experiments. Within the competing kinetics of a strain dependent activated incorporation of atoms and an asymmetry between upwards and downwards inter-layer migration, the model provides a consistent description of 2D versus 3D morphology evolution accompanied by the appearance of surface vacancies and steps at no energy cost. The correlated migration of these precursor defects offers an atomistic mechanism for the emergence of surface half-loops from the growth front (thus accounting for configurational and thermal entropy) governed by activation energies closer to their correlated motion under the evolving strain fields and thus substantially less than those calculated with respect to the perfect crystal as the reference state. The essential mechano-chemical nature of the problem is compared and contrasted with the historical literature of such phenomenon as precipitation hardening and sintering in metallic and ceramic composites.