Re Doping in 2D Transition Metal Dichalcogenides as a New Route to Tailor Structural Phases and Induced Magnetism

Alloying in 2D results in the development of new, diverse, and versatile systems with prospects in bandgap engineering, catalysis, and energy storage. Tailoring structural phase transitions using alloying is a novel idea with implications in designing all 2D device architecture as the structural phases in 2D materials such as transition metal dichalcogenides are correlated with electronic phases. Here, this study develops a new growth strategy employing chemical vapor deposition to grow monolayer 2D alloys of Re‐doped MoSe2 with show composition tunable structural phase variations. The compositions where the phase transition is observed agree well with the theoretical predictions for these 2D systems. It is also shown that in addition to the predicted new electronic phases, these systems also provide opportunities to study novel phenomena such as magnetism which broadens the range of their applications. Re doping is demonstrated to be a controllable way to tailor crystal structure and magnetic properties in chemical vapor deposition (CVD)‐synthesized 2D transition metal dichalcogenides. Extra electrons from Re atoms induce a 2H–1T′ phase transformation in monolayer Mo1–xRexSe2 alloys. These results show that chemical doping is a promising pathway to tune structural and magnetic properties of other CVD‐grown MX2 (M = Mo, W; X = S, Se).