Contact Geometry-Dependent Excitonic Emission in Mixed-Dimensional van der Waals Heterostructures

High Resolution Image Download MS PowerPoint Slide Manipulation of excitonic emission in two-dimensional (2D) materials via the assembly of van der Waals (vdW) heterostructures unlocks numerous opportunities for engineering their photonic and optoelectronic properties. In this work, we introduce a category of mixed-dimensional vdW heterostructures, integrating 2D materials with one-dimensional (1D) semiconductor nanowires composed of vdW layers. This configuration induces spatially distinct localized excitonic emissions through a tailored interfacial heterolayer atomic arrangement. By precisely adjusting both the axial and sidewall facet orientations of bottom-up grown PbI 2 vdW nanowires and by transferring them onto 1L WSe 2 flakes, we establish vdW heterointerfaces with either perpendicular or parallel interatomic arrangements. The edge-standing heterojunction, featuring perpendicular PbI 2 layers atop WSe 2, promotes efficient charge transfer through the edges and coupled localized states, leading to an enhanced redshifted excitonic emission. Conversely, the layer-by-layer heterointerface, where PbI 2 layers are in parallel contact with WSe 2, exhibits substantial quenching due to deep midgap states in a type-II alignment, as evidenced by power-dependent measurements and first-principle calculations. Our results introduce a method for actively manipulating excitonic emissions in 2D transition metal dichalcogenides (TMDs) through edge engineering, highlighting their potential in the development of various quantum devices.