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A method for growth of ultralarge grain (>100 μm) semiconductor thin-films on nonepitaxial substrates was developed via the thin-film vapor–liquid–solid growth mode. The resulting polycrystalline films exhibit similar optoelectronic quality as their single-crystal counterparts. Here, deterministic control of nucleation sites is presented by substrate engineering, enabling user-tuned internuclei spacing of up to ∼1 mm. Besides examining the theory associated with the nucleation process, this work presents an important advance toward controlled growth of high quality semiconductor thin films with unprecedented grain sizes on nonepitaxial substrates

Deterministic Nucleation of InP on Metal Foils with the Thin-Film Vapor–Liquid–Solid Growth Mode