Epitaxial composition-graded perovskite films grown by a dual-beam pulsed laser deposition method

We prepared SrTiO3 (STO) to Ba0.6Sr0.4TiO3 (BST06) out-of-plane composition-graded films on STO (100) substrates by means of a dual-beam dual-target pulsed laser deposition technique. In the deposition system, a sliding mirror divides one KrF excimer laser beam into two, realizing the dual-beam of controlled intensity ratio. X-ray diffraction reciprocal space mapping has revealed that the graded films deposited under oxygen pressure at or lower than 1×10−3mbar were coherently strained with the same in-plane lattice parameter as the substrate. Their composition gradient along the growth direction was confirmed by Rutherford backscattering analysis to be uniform. We deposited BST06 top layers of various thickness on epitaxial composition-graded (ECG) buffer layers and examined their coherency and crystallinity. In comparison with the cases of STO homoepitaxial buffer layers, ECG buffer layers achieved better crystallinity of top BST06 layers, suggesting that the crystallinity of a heteroepitaxially-grown film is affected not only by the in-plane lattice matching but also by the out-of-plane lattice continuity with the substrate. ECG films that bridge compositions of substrate and top layer materials can be useful buffer layers for epitaxial growth of lattice-mismatched oxide films. •Established a dual-beam pulsed laser deposition system with only one laser equipment.•Succeeded in growing coherently epitaxial composition graded perovskite-type titanate films.•Composition gradient was well controlled by carefully designing the mirror position sequence.•An epitaxial graded film is effective as a buffer layer to enhance the crystallinity of the top layer.