Nano-spectroscopy of excitons in atomically thin transition metal dichalcogenides

S. Zhang, B. Li, X. Chen, F. L. Ruta, Y. Shao, A. J. Sternbach, A. S. McLeod, Z. Sun, L. Xiong, S. L. Moore, X. Xu, W. Wu, S. Shabani, L. Zhou, Z. Wang, F. Mooshammer, E. Ray, N. Wilson, P. J. Schuck, C. R. Dean, A. N. Pasupathy, M. Lipson, X. Xu, X. Zhu, A. J. Millis, M. Liu, J. C. Hone and D. N. Basov

Nature Communications 13, 542 (2022)
Excitons play a dominant role in the optoelectronic properties of atomically thin van der Waals (vdW) semiconductors. These excitons are amenable to on-demand engineering with diverse control knobs, including dielectric screening, interlayer hybridization, and moiré potentials. However, external stimuli frequently yield heterogeneous excitonic responses at the nano- and meso-scales, making their spatial characterization with conventional diffraction-limited optics a formidable task. Here, we use a scattering-type scanning near-field optical microscope (s-SNOM) to acquire exciton spectra in atomically thin transition metal dichalcogenide microcrystals with previously unattainable 20 nm resolution. Our nano-optical data revealed material- and stacking-dependent exciton spectra of MoSe2, WSe2, and their heterostructures. Furthermore, we extracted the complex dielectric function of these prototypical vdW semiconductors. s-SNOM hyperspectral images uncovered how the dielectric screening modifies excitons at length scales as short as few nanometers. This work paves the way towards understanding and manipulation of excitons in atomically thin layers at the nanoscale.