Thick epitaxial BaTiO3 films ranging from 120 nm to 1 μm were grown by off-axis RF magnetron sputtering on SrTiO3-templated silicon-on-insulator (SOI) substrates for use in electro-optic applications, where such large thicknesses are necessary. The films are of high quality, rivaling those grown by molecular beam epitaxy (MBE) in crystalline quality, but can be grown 10 times faster. Extraction of lattice parameters from geometric phase analysis of atomic-resolution scanning transmission electron microscopy images revealed how the in-plane and out-of-plane lattice spacings of sputtered BaTiO3 changes as a function of layer position within a thick film. Our results indicate that compared to molecular beam epitaxy, sputtered films retain their out-of-plane polarization (c-axis) orientation for larger thicknesses. We also find an unusual re-transition from in-plane polarization (a-axis) to out-of-plane polarization (c-axis), along with an anomalous lattice expansion, near the surface. We also studied a method of achieving 100% a-axis-oriented films using a two-step process involving amorphous growth and recrystallization of a seed layer followed by normal high temperature growth. While this method is successful in achieving full a-axis orientation even at low thicknesses, the resulting film has a large number of voids and misoriented grains. Electro-optic measurement using a transmission setup of a sputtered BTO film grown using the optimized conditions yields an effective Pockels coefficient as high as 183 pm/V. A Mach-Zehnder modulator fabricated on such films exhibits phase shifting with an equivalent Pockels coefficient of 157 pm/V. These results demonstrate that sputtered BTO thick films can be used for integrated electro-optic modulators for Si photonics.
Keywords: barium titanate; electro-optic modulator; epitaxial growth; off-axis sputtering; pockels effect; silicon photonics; waveguides.