Realization of polytype heterostructures via delicate structural transitions from a doped-Mott insulator

Transition metal dichalcogenides (TMDs) host multiple competing structural and electronic phases, making them an ideal platform for constructing polytype heterostructures with emergent quantum properties. However, controlling phase transitions to form diverse heterostructures inside a single crystal remains challenging. Here, we realize vertical/lateral polytype heterostructures in a hole-doped Mott insulator via thermal-annealing-induced structural transitions. Raman spectroscopy, atomic force microscopy (AFM) and scanning Kelvin probe force microscopy (SKPM) confirm the coexistence of T-H polytype heterostructures. Atomic-scale scanning tunneling microscopy/spectroscopy (STM/STS) measurements reveal the transparent effect in 1H/1T vertical heterostructures, where positive bias voltage induces in a pronounced superposition of the √13×√13 CDW of the 1T-layer on the 1H-layer. By systematically comparing 1T/1H and 1T/1T interfaces, we demonstrate that the metallic 1H-layer imposes a Coulomb screening effect on the 1T-layer, suppressing the formation of CDW domain walls and forming more ordered electronic states. These results clarify the interfacial coupling between distinct quantum many-body phases and establish a controllable pathway for constructing two-dimensional polytype heterostructures with tunable electronic properties.