Quasi‐Continuous Tuning of Carrier Polarity in Monolayered Molybdenum Dichalcogenides through Substitutional Vanadium Doping

Abstract Semiconducting 2D transition metal dichalcogenides (2D TMDs) with tunable electronic properties are a fundamental prerequisite for the development of next generation advanced electronic/optoelectronic devices. However, controllable and quasi‐continuous tuning carrier polarity of monolayered MoS 2 ranging from intrinsic n ‐type to p ‐type via ambipolarity still remains a challenge. Herein, quasi‐continuous tailoring of carrier polarity of monolayered MoS 2 through substitutional doping of molybdenum (Mo) with vanadium (V) atoms is presented. Atomic distribution in real space characterized by spherical aberration‐corrected scanning transmission electron microscopy (Cs‐STEM) reveals that the V atoms randomly substitute Mo in monolayered MoS 2 , and its doping concentration can be tuned in a wide range from 0.7 to ≈10 at.%. Electrical measurements confirm that the carrier polarity of the monolayered MoS 2 can be tuned from intrinsic n ‐type to p ‐type via ambipolarity depending on the V doping degree, consistent with the density functional theory calculations. Moreover, this doping strategy is demonstrated to extend to other monolayered 2D TMDs by using MoSe 2 as a model material, owing to a good universality.