Visualization of Band Shifting and Interlayer Coupling in WxMo1- xS2 Alloys Using Near-Field Broadband Absorption Microscopy

ACS Nano. 2022 May 24;16(5):7503-7511. doi: 10.1021/acsnano.1c10593. Epub 2022 Apr 29.

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.

Keywords: WxMo1−xS2 alloy; band shifting; broadband absorption microscopy; interlayer coupling; scanning near-field optical microscopy (SNOM).