Strain-Induced Metastable Topological Networks in Laser-Fabricated TaS(2) Polytype Heterostructures for Nanoscale Devices

[Image: see text] The stacking of layered materials into heterostructures offers diverse possibilities for generating deformed moiré states arising from their mutual interaction. Here we report self-assembled two-dimensional nanoscale strain networks formed within a single prismatic (H) polytype monolayer of TaS(2) created in situ on the surface of an orthorhombic 1T-TaS(2) single crystal by a low-temperature laser-induced polytype transformation. The networks revealed by scanning tunneling microscopy (STM) take on diverse configurations at different temperatures, including extensive double stripes and a twisted 3-gonal mesh of connected 6-pronged vertices. The resulting phase diagram can be understood to be a consequence of thermally driven minimization of discommensurations between the H and 1T layers. Nontrivial dislocation defects of embedded 2- and 4-gonal structures are shown to be associated with local inhomogeneous strains. The creation of metastable heterostructures by laser quench at cryogenic temperatures in combination with STM manipulation of local strain demonstrates nanoscale control of topological defects in transition metal dichalcogenide heterostructures may be utilized in the fabrication of nanoscale electronic devices and neural networks.