Distinct Nucleation and Growth Kinetics of Amorphous SrTiO₃ on (001) SrTiO₃ and SiO₂/Si: A Step toward New Architectures

Integration of emerging complex-oxide compounds into sophisticated nanoscale single-crystal geometries faces significant challenges arising from the kinetics of vapor-phase thin-film epitaxial growth. A comparison of the crystallization of the model perovskite SrTiO3 (STO) on (001) STO and oxidized (001) Si substrates indicates that there is a viable alternative route that can yield three-dimensional epitaxial synthesis, an approach in which STO is crystallized from an amorphous thin film by postdeposition annealing. The crystallization of amorphous STO on single-crystal (001) STO substrates occurs via solid-phase epitaxy (SPE), without nucleation and with a temperature-dependent amorphous/crystalline interface velocity. In comparison, the crystallization of STO on SiO2/(001) Si substrates requires nucleation, resulting in a polycrystalline film with crystal sizes on the order of 10 nm. A comparison of the temperature dependence of the nucleation and growth processes for these two substrates indicates that it will be possible to create crystalline STO materials using low-temperature crystallization from a crystalline seed, even in the presence of interfaces with other materials. These processes provide a potential route for the formation of single crystals with intricate three-dimensional nanoscale geometries.