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Mcclimon, John Brandon
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article
Synthesis and Physical Properties of Phase-Engineered Transition Metal Dichalcogenide Monolayer Heterostructures
Abstract
Heterostructures of transition metal dichalcogenides (TMDs) offer the attractive prospect of combining distinct physical properties derived from different TMD structures. Here, we report direct chemical vapor deposition of in-plane monolayer heterostructures based on 1H-MoS<sub>2</sub> and 1T′-MoTe<sub>2</sub>. The large lattice mismatch between these materials led to intriguing phenomena at their interface. Atomic force microscopy indicated buckling in the 1H region. Tip-enhanced Raman spectroscopy showed mode structure consistent with Te substitution in the 1H region during 1T′-MoTe<sub>2</sub> growth. This was confirmed by atomic resolution transmission electron microscopy, which also revealed an atomically stitched, dislocation-free 1H/1T′ interface. Theoretical modeling revealed that both the buckling and absence of interfacial misfit dislocations were explained by lateral gradients in Te substitution levels within the 1H region and elastic coupling between 1H and 1T′ domains. Phase field simulations predicted 1T′ morphologies with spike-shaped islands at specific orientations consistent with experiments. Electrical measurements across the heterostructure confirmed its electrical continuity. This work demonstrates the feasibility of dislocation-free stitching of two different atomic configurations and a pathway toward direct synthesis of monolayer TMD heterostructures of different phases.