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This study constructed the Zr2CTx–MoS2 vdW-HS and focused on discussing the modulation mechanisms and trends of the SBH in this system under the influence of different functional group types (−F/–O/–OH) and concentration gradients (0%, 25%, 50%, 75%, 100%). Phonon spectrum and interfacial binding energy calculations revealed that all structures possess stability. Systems with >50% −O concentration exhibited bandgaps, enabling heterojunction bandgap modulation between 0.02 and 1.35 eV. Opposite trends emerged between n-type (Φe) and p-type (Φh) SBH: in −O systems, increasing −O concentration progressively decreased Φh while increasing Φe, yielding maximum/minimum Φe values of 0.668/–0.362 eV and Φh values of 1.366/0.418 eV. Systems with −OH doped into −F configurations exhibited stable SBH variations, with n-type Ohmic contacts emerging repeatedly during functional group doping and tuning processes. These phenomena originate from doping-induced work function changes (2.0–4.3 eV range), where altered work function differences drive interfacial charge redistribution. This subsequently modulates the direction and magnitude of MoS2 band bending, ultimately shifting its CBM and VBM to achieve SBH control. These findings provide a theoretical basis for designing and optimizing high-performance two-dimensional semiconductor devices that are more miniaturized and have lower contact resistance.
Hou et al. (Wed,) studied this question.