Type-II Interface Band Alignment in the vdW PbI₂-MoSe₂ Heterostructure

Energy band alignments at heterostructure interfaces play key roles in device performance, especially between two-dimensional atomically thin materials. Herein, van der Waals PbI₂-MoSe₂ heterostructures fabricated by in situ PbI₂ deposition on monolayer MoSe₂ are comprehensively studied using scanning tunneling microscopy/spectroscopy, atomic force microscopy, photoemission spectroscopy, and Raman and photoluminescence (PL) spectroscopy. PbI₂ grows on MoSe₂ in a quasi layer-by-layer epitaxial mode. A type-II interface band alignment is proposed between PbI₂ and MoSe₂ with the conduction band minimum (valence band maximum) located at PbI₂ (MoSe₂), which is confirmed by first-principles calculations and the existence of interfacial excitons revealed using temperature-dependent PL. Our findings provide a scalable method to fabricate PbI₂-MoSe₂ heterostructures and new insights into the electronic structures for future device design.