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Abstract

Epitaxial growth of two-dimensional (2D) materials with uniform orientation has been previously realized by introducing a small binding energy difference between the two locally most stable orientations. However, this small energy difference can be easily disturbed by uncontrollable dynamics during the growth process, limiting its practical applications. Herein, we propose a quasi-equilibrium growth (QEG) strategy to synthesize inch-scale monolayer α-In₂Se₃ single crystals, a semiconductor with ferroelectric properties, on fluor-phlogopite substrates. The QEG facilitates the discrimination of small differences in binding energy between the two locally most stable orientations, realizing robust single-orientation epitaxy within a broad growth window. Thus, single-crystal α-In₂Se₃ film can be epitaxially grown on fluor-phlogopite, the cleavage surface atomic layer of which has the same 3-fold rotational symmetry with α-In₂Se₃. The resulting crystalline quality enables high electron mobility up to 117.2 cm² V⁻¹ s⁻¹ in α-In₂Se₃ ferroelectric field-effect transistors, exhibiting reliable nonvolatile memory performance with long retention time and robust cycling endurance. In brief, the developed QEG method provides a route for preparing larger-area single-crystal 2D materials and a promising opportunity for applications of 2D ferroelectric devices and nanoelectronics.