Mobility Optimization in LaxBa1-xSnO3 Thin Films Deposited via High Pressure Oxygen Sputtering

Abstract

BaSnO3 (BSO) is one of the most promising semiconducting oxides currently being explored for use in future electronic applications. BSO possesses a unique combination of high room temperature mobility (even at very high carrier concentrations, >1019 cm-3), wide band gap, and high temperature stability, making it a potentially useful material for myriad applications. Significant challenges remain however in optimizing the properties and processing of epitaxial BSO, a critical step towards industrial applications. In this study we investigate the viability of using high pressure oxygen sputtering to produce high mobility La-doped BSO thin films. In the first part of our investigation we synthesized, using solid state reaction, phase-pure stoichiometric polycrystalline 2% La-doped BaSnO3 for use as a target material in our sputtering system. We verified the experimental bulk lattice constant, 4.117 Å, to be in good agreement with literature values. Next, we set out to optimize the growth conditions for DC sputtering of La doped BaSnO3. We found that mobility for all our films increased monotonically with deposition temperature, suggesting the optimum temperature for deposition is >900°C and implicating a likely improvement in transport properties with post-growth thermal anneal. We then preformed systematic studies aimed at probing the effects of varying thickness and deposition rate to optimize the structural and electronic transport properties in unbuffered BSO films. In this report we demonstrate the ability to grow 2% La BSO thin films with an effective dopant activation of essentially 100%. Our films showed fully relaxed (bulk), out-of-plane lattice parameter values when deposited on LaAlO3, MgO, and (LaAlO3)0.3(Sr2TaAlO6)0.7 substrates, and slightly expanded out-of-plane lattice parameters for films deposited on SrTiO3, GdScO3, and PrScO3 substrates. The surface roughness’s of our films were measured via AFM, and determined to be on the nm scale or better. Specular XRD measurements confirmed highly crystalline films with narrow rocking curve FWHMs on the order of 0.05°. The optimum thickness found to maximize mobility was around 100 nm for films deposited at ~8 Å/min. These films exhibited room temperature mobilities in excess of 50 cm2V-1s 1 at carrier concentrations ~3 x 1020 cm-3 across 4 different substrate materials (LaAlO3, SrTiO3, GdScO3, and PrScO3). Contrary to expectations, our findings showed no dependence of mobility on substrate mismatch, indicating that threading dislocations are either not the dominant scattering source, or that threading dislocation density in the films was constant regardless of the substrate. The highest mobility film achieved in this study, 70 cm2V 1s 1, was measured for a film grown at a considerably slower rate (~2 Å/min) and lower thickness (~380 Å). Said film was deposited on a PrScO3 (110) substrate, the most closely lattice matched substrate commercially available for BSO (–2.2% pseudo-cubic). This film showed a high out-of-plane lattice parameter from X-ray diffraction (aop = 4.158 Å), suggesting a significantly strained film. This result highlights the possibility of sputtering coherent, fully strained, BSO films, far exceeding the theoretical critical thickness for misfit dislocation formation, on closely lattice matched substrates. Overall, this work validates the concept of high pressure oxygen sputtering to produce high mobility La-doped BSO films. The mobility values reported in this thesis are comparable to those found for films deposited via pulsed laser deposition in previous studies, and represent record values for sputter deposited BSO thin films.