Thermally Induced 2D Alloy-Heterostructure Transformation in Quaternary Alloys

Composition and phase specific 2D transition metal dichalogenides (2D TMDs) with a controlled electronic and chemical structure are essential for future electronics. While alloying allows bandgap tunability, heterostructure formation creates atomically sharp electronic junctions. Herein, the formation of lateral heterostructures from quaternary 2D TMD alloys, by thermal annealing, is demonstrated. Phase separation is observed through photoluminescence and Raman spectroscopy, and the sharp interface of the lateral heterostructure is examined via scanning transmission electron microscopy. The composition-dependent transformation is caused by existence of miscibility gap in the quaternary alloys. The phase diagram displaying the miscibility gap is obtained from the reciprocal solution model based on density functional theory and verified experimentally. The experiments show direct evidence of composition-driven heterostructure formation in 2D atomic layer systems.