Scalable Substitutional Re‐Doping and its Impact on the Optical and Electronic Properties of Tungsten Diselenide

Reliable, controlled doping of 2D transition metal dichalcogenides will enable the realization of next-generation electronic, logic-memory, and magnetic devices based on these materials. However, to date, accurate control over dopant concentration and scalability of the process remains a challenge. Here, a systematic study of scalable in situ doping of fully coalesced 2D WSe₂ films with Re atoms via metal-organic chemical vapor deposition is reported. Dopant concentrations are uniformly distributed over the substrate surface, with precisely controlled concentrations down to <0.001% Re achieved by tuning the precursor partial pressure. Moreover, the impact of doping on morphological, chemical, optical, and electronic properties of WSe₂ is elucidated with detailed experimental and theoretical examinations, confirming that the substitutional doping of Re at the W site leads to n-type behavior of WSe₂ . Transport characteristics of fabricated back-gated field-effect-transistors are directly correlated to the dopant concentration, with degrading device performances for doping concentrations exceeding 1% of Re. The study demonstrates a viable approach to introducing true dopant-level impurities with high precision, which can be scaled up to batch production for applications beyond digital electronics.