Self-organized formation of step-terrace structure in SrRuO3 thin films grown on mixed-terminated SrTiO3 (100) substrates

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Surface morphology of the substrate and bottom layers plays a critical role in the epitaxial growth of oxide thin films. Here, we report on the self-organized formation of a step-terrace structure in SrRuO3 (SRO) thin films grown using pulsed laser deposition on mixed-terminated SrTiO3 (100) substrates without any prior surface treatment. Atomic force microscopy observations reveal that SRO films initially grow in a three-dimensional island mode and subsequently undergo a transition to a step-flow growth mode through island coalescence as the film thickness increases, resulting in a well-defined step-terrace morphology with a step height consistent with the SRO unit-cell parameter. The average terrace width of the self-organized structure can be systematically tuned by varying the substrate temperature and the target-substrate distance, which we attribute to changes in the critical island radius that governs the nucleation behavior. To demonstrate the utility of this self-organized morphology, we show that BiFeO3 thin films grown on SRO films with such a step-terrace structure exhibit improved surface flatness and crystalline quality compared to those grown directly on bare SrTiO3 substrates. These findings provide a clear understanding of the mechanism of thickness-driven growth-mode transitions in perovskite oxide thin films under various growth conditions.