Phase-selective in-plane heteroepitaxial growth of H-phase CrSe₂

Phase engineering of two-dimensional transition metal dichalcogenides (2D-TMDs) offers opportunities for exploring unique phase-specific properties and achieving new desired functionalities. Here, we report a phase-selective in-plane heteroepitaxial method to grow semiconducting H-phase CrSe₂. The lattice-matched MoSe₂ nanoribbons are utilized as the in-plane heteroepitaxial template to seed the growth of H-phase CrSe₂ with the formation of MoSe₂-CrSe₂ heterostructures. Scanning tunneling microscopy and non-contact atomic force microscopy studies reveal the atomically sharp heterostructure interfaces and the characteristic defects of mirror twin boundaries emerging in the H-phase CrSe₂ monolayers. The type-I straddling band alignments with band bending at the heterostructure interfaces are directly visualized with atomic precision. The mirror twin boundaries in the H-phase CrSe₂ exhibit the Tomonaga-Luttinger liquid behavior in the confined one-dimensional electronic system. Our work provides a promising strategy for phase engineering of 2D TMDs, thereby promoting the property research and device applications of specific phases.