Sequential pulsed laser deposition of homoepitaxial SrTiO3 thin films

The control of thin film stoichiometry is of primary relevance to achieve desired functionality. Pulsed laser deposition ablating from binary-oxide targets (sequential deposition) can be applied to precisely control the film composition, offsetting the importance of growth conditions on the film stoichiometry. In this work, we demonstrate that the cation stoichiometry of SrTiO3 thin films can be finely tuned by sequential deposition from SrO and TiO2 targets. Homoepitaxial SrTiO3 films were deposited at different substrate temperatures and Ti/Sr pulse ratios, allowing the establishment of a growth window for stoichiometric SrTiO3. The growth kinetics and nucleation processes were studied by reflection high-energy electron diffraction and atomic force microscopy, providing information about the growth mode and the degree of off-stoichiometry. At the optimal (stoichiometric) growth conditions, films exhibit atomically flat surfaces, whereas off-stoichiometry is accommodated by crystal defects, 3D islands, and/or surface precipitates depending on the substrate temperature and the excess cation. This technique opens the way to precisely control stoichiometry and doping of oxide thin films. Published by AIP Publishing.