Substrate influence on transition metal dichalcogenide monolayer exciton absorption linewidth broadening

TL;DR

This study investigates how different substrates and encapsulation materials affect exciton absorption linewidth broadening in TMD monolayers, highlighting the roles of roughness, cleanliness, and charge trapping, with extit{h}-BN being most effective.

Contribution

It provides a detailed analysis of substrate and encapsulation effects on linewidth broadening in TMDs using EELS and diffraction, emphasizing extit{h}-BN's advantages.

Findings

Monolayer roughness significantly affects linewidth broadening.

Surface cleanliness reduces inhomogeneous broadening.

extit{h}-BN minimizes charge disorder and protects against damage.

Abstract

The excitonic states of transition metal dichacolgenide (TMD) monolayers are heavily influenced by their external dielectric environment based on the substrate used. In this work, various wide bandgap dielectric materials, namely hexagonal boron nitride (\textit{h}-BN) and amorphous silicon nitride (Si$_3$N$_4$), under different configurations as support or encapsulation material for WS$_2$ monolayers are investigated to disentangle the factors contributing to inhomogeneous broadening of exciton absorption lines in TMDs using electron energy loss spectroscopy (EELS) in a scanning transmission electron microscope (STEM). In addition, monolayer roughness in each configuration was determined from tilt series of electron diffraction patterns by assessing the broadening of diffraction spots by comparison with simulations. From our experiments, the main factors that play a role in linewidth broadening can be classified in increasing order of importance by: monolayer roughness, surface cleanliness, and substrate-induced charge trapping. Furthermore, because high-energy electrons are used as a probe, electron beam-induced damage on bare TMD monolayer is also revealed to be responsible for irreversible linewidth increases. \textit{h}-BN not only provides clean surfaces of TMD monolayer, and minimal charge disorder, but can also protect the TMD from irradiation damage. This work provides a better understanding of the mechanisms by which \textit{h}-BN remains, to date, the most compatible material for 2D material encapsulation, facilitating the realization of intrinsic material properties to their full potential.