Combinatorial synthesis of heteroepitaxial, multi-cation, thin-films via pulsed laser deposition coupled with in-situ, chemical and structural characterization

Combinatorial synthesis via a continuous composition spread is an excellent route to develop thin-film libraries as it is both time- and cost-efficient. Creating libraries of functional, multicomponent, complex oxide films requires excellent control over the synthesis parameters combined with high-throughput analytical feedback. A reliable, high-throughput, in-situ characterization analysis method is required to meet the crucial need to rapidly screen materials libraries. Here, we report on the combination of two in-situ techniques—(a) Reflection high-energy electron diffraction (RHEED) for heteroepitaxial characterization and a newly developed compositional analysis technique, low-angle x-ray spectroscopy (LAXS), to map the chemical composition profile of combinatorial heteroepitaxial complex oxide films deposited using a continuous composition spread method via pulsed laser deposition. This is accomplished using a unique state-of-the-art combinatorial growth system with a fully synchronized four-axis mechanical substrate stage without shadow masks, alternating acquisition of chemical compositional data using LAXS at various different positions on the [Formula: see text] 41 mm [Formula: see text] 41 mm range and sequential deposition of multilayers of SrTiO[Formula: see text] and [Formula: see text] on a 2-inch (50.8 mm) [Formula: see text] wafer in a single growth run. Rutherford backscattering spectrometry (RBS) is used to calibrate and validate the compositions determined by LAXS. This study shows the feasibility of combinatorial synthesis of heteroepitaxial, functional complex oxide films at wafer-scale via two essential in-situ characterization tools—RHEED for structural analysis or heteroepitaxy and LAXS for compositional characterization. This is a powerful technique for development of new films with optimized heteroepitaxy and composition.