Molten‐Salt‐Assisted Chemical Vapor Deposition Process for Substitutional Doping of Monolayer MoS(2) and Effectively Altering the Electronic Structure and Phononic Properties

Substitutional doping of layered transition metal dichalcogenides (TMDs) has been proved to be an effective route to alter their intrinsic properties and achieve tunable bandgap, electrical conductivity and magnetism, thus greatly broadening their applications. However, achieving valid substitutional doping of TMDs remains a great challenge to date. Herein, a distinctive molten‐salt‐assisted chemical vapor deposition (MACVD) method is developed to match the volatilization of the dopants perfectly with the growth process of monolayer MoS(2), realizing the substitutional doping of transition metal Fe, Co, and Mn. This doping strategy effectively alters the electronic structure and phononic properties of the pristine MoS(2). In addition, a temperature‐dependent Raman spectrum is employed to explore the effect of dopants on the lattice dynamics and first‐order temperature coefficient of monolayer MoS(2), and this doping effect is illustrated in depth combined with the theoretical calculation. This work provides an intriguing and powerful doping strategy for TMDs through employing molten salt in the CVD system, paving the way for exploring new properties of 2D TMDs and extending their applications into spintronics, catalytic chemistry and photoelectric devices.