Band alignment engineering is crucial and feasible to enrich the functionalities of van der Waals heterojunctions (vdWHs) for rectifying functions in next-generation information storage technologies. However, band alignment tunability is volatile as it needs a sustained external field to maintain the Femi level of single components, which hinders the implementation of nonvolatile functions. Here, the ferroelectric semiconducting nature of alpha-In2Se3 is utilized to design vdWHs based on two-dimensional transition metal dichalcogenides (TMDs)/alpha-In2Se3, where TMDs are used as the channel, and the ferroelectric semiconductor alpha-In2Se3 is assembled as an asymmetric gate. A density functional theory validates that the band offset in a homogeneous TMDs channel is tuned by coupling the effect of the semiconducting nature and asymmetric ferroelectric gate of alpha-In2Se3, which induces simultaneous rectifying and memory functions. This includes a programmable rectifying ratio of up to 104, ultra-large memory window (110 V), programming/erasing of 104, and good endurance. The tuned band offset from the asymmetric ferroelectric semiconductor gate is conceptualized as a guideline to realize a simultaneous rectifying and memory device with high programmability.
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