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Semiconductor heterostructures are the fundamental platform for manyimportant device applications such as lasers, light-emitting diodes, solarcells and high-electron-mobility transistors. Analogous to traditionalheterostructures, layered transition metal dichalcogenide (TMDC)heterostructures can be designed and built by assembling individualsingle-layers into functional multilayer structures, but in principle withatomically sharp interfaces, no interdiffusion of atoms, digitally controlledlayered components and no lattice parameter constraints. Nonetheless, theoptoelectronic behavior of this new type of van der Waals (vdW) semiconductorheterostructure is unknown at the single-layer limit. Specifically, it isexperimentally unknown whether the optical transitions will be spatially director indirect in such hetero-bilayers. Here, we investigate artificialsemiconductor heterostructures built from single layer WSe2 and MoS2 buildingblocks. We observe a large Stokes-like shift of ~100 meV between thephotoluminescence peak and the lowest absorption peak that is consistent with atype II band alignment with spatially direct absorption but spatially indirectemission. Notably, the photoluminescence intensity of this spatially indirecttransition is strong, suggesting strong interlayer coupling of charge carriers.The coupling at the hetero-interface can be readily tuned by insertinghexagonal BN (h-BN) dielectric layers into the vdW gap. The generic nature ofthis interlayer coupling consequently provides a new degree of freedom in bandengineering and is expected to yield a new family of semiconductorheterostructures having tunable optoelectronic properties with customizedcomposite layers.

Strong interlayer coupling in van der Waals heterostructures built from single-layer chalcogenides