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构建范德瓦耳斯异质结是丰富二维材料物性并增强其光电等性能的有效策略。本文基于第一性原理模拟，系统研究了两种不同界面结构的Janus MoSSe/g-C3N4异质结（即SMoSe/g-C3N4和SeMoS/g-C3N4）的电子性质及其双轴应变调控规律。结果表明，针对SMoSe/g-C3N4异质结构，MoSSe本征偶极场与界面电场方向一致，相互叠加形成由g-C3N4指向MoSSe的增强电场，体系呈现I型能带排列特征；而在SeMoS/g-C3N4异质结构中，两者方向相反，部分相互抵消后形成由MoSSe指向g-C3N4的净电场，呈现II型能带排列特征，可促进载流子的分离从而有效提升其光催化分解水活性。进一步研究发现，施加双轴应变可有效调节两种异质结构的电子能带，尤其在SeMoS/g-C3N4中可实现I型与II型能带结构的可逆转变。本研究为Janus MoSSe/g-C3N4异质结在光催化与光电器件领域的应用提供了理论依据。Constructing van der Waals (vdW) heterostructures has emerged as an effective strategy for enriching the physical properties of two-dimensional materials and optimizing their optoelectronic performance. In this work, we systematically investigate the electronic properties and biaxial strain modulation of Janus MoSSe/g-C3N4 heterostructures with two distinct interfacial configurations—SMoSe/g-C3N4 and SeMoS/g-C3N4—by means of first-principles simulations. The binding energy comparison and AIMD simulations were performed in order to determine the most stable stacking pattern of each type of the heterostructure. Analysis of the electrostatic potential and work function shows that the intrinsic dipole of MoSSe layer and the interfacial electric field in the SMoSe/g-C3N4 heterostructure exhibit a constructive superposition, enhancing the overall built-in electric field pointing from g-C3N4 to MoSSe layer, and resulting in a type-I band alignment. In contrast, in the SeMoS/g-C3N4 configuration, the two fields oppose each other, leading to a net electric field directed from MoSSe to g-C3N4 layer and thus a type-II band alignment, which facilitates spatial carrier separation and significantly improves the photocatalytic water-splitting activity. Furthermore, this study also demonstrates that biaxial strain can effectively modulate the electronic band structures of both types of heterostructures. In particular, the SeMoS/g-C3N4 system exhibits a reversible transition between type-I and type-II band alignments under specific compressive (-4%) and tensile (+5%) strain states. The underline mechanism is elucidated by the difference charge density calculations. This study provides theoretical insights into the role of interfacial and intrinsic dipoles coupled with strain engineering, offering a viable route for designing efficient MoSSe/g-C3N4-based photocatalysts and optoelectronic devices.
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Keywords:
- heterostructure /
- electronic band structure /
- strain engineering /
- first-principles simulations
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