Abstract

AbstractSemiconducting 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 MoS2 ranging from intrinsic n‐type to p‐type via ambipolarity still remains a challenge. Herein, quasi‐continuous tailoring of carrier polarity of monolayered MoS2 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 MoS2, 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 MoS2 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 MoSe2 as a model material, owing to a good universality.

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