Probing Exciton Complexes and Charge Distribution in Inkslab-Like WSe₂ Homojunction

By virtue of the layer-dependent band structure and valley-selected optical/electronic properties, atomically layered transition-metal dichalcogenides (TMDs) exhibit great potentials such as in valleytronics and quantum devices, and have captured significant attentions. Precise control of the optical and electrical properties of TMDs is always the pursuing goal for real applications, and constructing advanced structures that allow playing with more degrees of freedom may hold the key. Here, we introduce a triangular inkslab-like WSe₂ homojunction with a monolayer in the inner surrounded by a multilayer frame. Benefit from this interesting structure, the photoluminescence (PL) peaks redshift up to 50 meV and the charge density increases about 6 times from the center to the edge region of the inner monolayer. We demonstrated that the Se-deficient multilayer frame offers the excessive free electrons for the generation of the electron density gradient inside the monolayer, which also results in the spatial variation and distribution gradient of a series of exciton complexes. Furthermore, we observed the strong rectifying characteristic and clear photovoltaic response across the homojunction through measuring and mapping the photocurrent of the devices. Our result provides another route for efficient modulation of the exciton-complex emissions of TMDs, which is exceptionally desirable for the "layer- and charge-engineered" photonic and optoelectronic devices.