ABSTRACT
Beyond-diffraction-limit optical absorption spectroscopy provides in-depth information on the graded band structures of composition-spread and stacked two-dimensional materials, in which direct/indirect bandgap, interlayer coupling, and defects significantly modify their optoelectronic functionalities such as photoluminescence efficiency. We here visualize the spatially varying band structure of monolayer and bilayer transition metal dichalcogenide alloys by using near-field broadband absorption microscopy. The near-field spectral and spatial information manifests the excitonic band shift that results from the interplay of composition spreading and interlayer coupling. These results enable us to identify, notably, the top layer of the bilayer alloy as pure WS2. We also use the aberration-free near-field transmission images to demarcate the exact boundaries of alloyed and pure transition metal dichalcogenides. This technology can offer valuable insights on various layered structures in the era of "stacking science" in the quest of quantum optoelectronic devices.
ABSTRACT
Heterojunctions made by laterally stitching two different transition metal dichalcogenide monolayers create a unique one-dimensional boundary with intriguing local optical properties that can only be characterized by nanoscale-spatial-resolution spectral tools. Here, we use near-field photoluminescence (NF-PL) to reveal the narrowest region (105 nm) ever reported of photoluminescence quenching at the junction of a laterally stitched WS2/MoS2 monolayer. We attribute this quenching to the atomically sharp band offset that generates a strong electric force at the junction to easily dissociate excitons. Besides the sharp heterojunction, a model considering various widths of the alloying interfacial region under low or high optical pumping is presented. With a spatial resolution six times better than that of confocal microscopy, NF-PL provides an unprecedented spectral tool for non-scalable 1D lateral heterojunctions.
