Two-dimensional solid-phase crystallization toward centimeter-scale monocrystalline layered MoTe₂: Via two-step annealing

The lack of effective synthesis techniques for achieving wafer-scale uniformity and high crystallinity remains one of the major obstacles for two-dimensional (2D) layered materials in practical applications. 2D solid-phase crystallization (2DSPC) is proposed based on the area-scalable and semiconductor-process-compatible sputtering and thermal annealing techniques. It successfully synthesizes few-layer 2H-MoTe2 with a monocrystalline grain size exceeding half a centimeter on an amorphous substrate of silicon dioxide. The extremely large grain size is made possible through a two-step annealing process in an inert atmosphere. The initial rapid thermal annealing at high temperatures produces hexagonal monocrystalline 2H-MoTe2 seeds with low density and the subsequent long-duration furnace annealing at low temperatures enlarges the monocrystalline domains only from the pre-existing seeds. The 2DSPC mechanism and its morphological evolution agree with the classical nucleation theory and kinetic Wulff construction theory, respectively. Our result suggests the promising potential of 2DSPC as a simple yet effective route for synthesizing future wafer-scale, high-quality 2D materials.