Self-Healing Originated van der Waals Homojunctions with Strong Interlayer Coupling for High-Performance Photodiodes

The dangling-bond-free surfaces of van der Waals (vdW) materials make it possible to build ultrathin junctions. Fundamentally, the interfacial phenomena and related optoelectronic properties of vdW junctions are modulated by the interlayer coupling effect. However, the weak interlayer coupling of vdW heterostructures limits the interlayer charge transfer efficiency, resulting in low photoresponsivity. Here, a bilayer MoS₂ homogeneous junction is constructed by stacking the as-grown onto the self-healed monolayer MoS₂. The homojunction barrier of ∼165 meV is obtained by the electronic structure modulation of defect self-healing. This homojunction reveals the stronger interlayer coupling effect in comparison with vdW heterostructures. This ultrastrong interlayer coupling effect is experimentally verified by Raman spectra and angle-resolved photoemission spectroscopy. The ultrafast interlayer charge transfer takes place within ∼447 fs, which is faster than those of most vdW heterostructures. Furthermore, the homojunction photodiode manifests outstanding rectifying behavior with an ideal factor of ∼1.6, perfect air stability over 12 months, and high responsivity of ∼54.6 mA/W. Moreover, the interlayer exciton peak of ∼1.66 eV is found in vdW homojunctions. This work offers an uncommon vdW junction with strong interlayer coupling and perfects the relevance of interlayer coupling and interlayer charge transfer.