Probing dark exciton navigation through a local strain landscape in a WSe$_2$ monolayer

TL;DR

This study develops a cryogenic nanoscale strain technique to investigate dark and bright exciton dynamics in WSe$_2$ monolayers, revealing dark excitons' role in strain-guided exciton transport at cryogenic temperatures.

Contribution

It introduces a novel nanosculpted fiber method to probe exciton behavior in strained TMD monolayers, especially focusing on dark excitons' dynamics and their influence on exciton transport.

Findings

Dark excitons are funneled to high-strain regions during their long lifetime.

Strain causes a significant red shift in photoluminescence peaks, up to 390 meV.

Dark excitons dominate drift and diffusion at cryogenic temperatures.

Abstract

Monolayers of transition metal dichalcogenides (TMDs) have recently emerged as a promising optoelectronic platform. To leverage their full potential, however, it is important to understand and engineer the properties of the different exciton species that exist in these monolayers, as well as to control their transport through the material. A promising approach relies on engineering strain landscapes in atomically thin semiconductors that excitons navigate. In WSe$_2$ monolayers, for example, localized strain has been used to control the emission wavelength of excitons, induce exciton funneling and conversion, and even realize single-photon sources and quantum dots. Before these phenomena can be fully leveraged for applications, including quantum information processing, the details of excitons' interaction with the strain landscape must be well understood. To address this, we have developed a cryogenic technique capable of probing the dynamics of both bright and dark excitons in nanoscale strain landscapes in TMDs. In our approach, a nanosculpted tapered optical fiber is used to simultaneously generate strain and probe the near-field optical response of WSe$_2$ monolayers at 5 K. When the monolayer is pushed by the fiber, its lowest energy photoluminescence (PL) peaks red shift by as much as 390 meV, (corresponding to 20% of the bandgap of an unstrained WSe$_2$ monolayer). The red-shifting peaks are polarized perpendicularly to the WSe$_2$ plane and have long rising times (10 ps) and lifetimes (52 ps), indicating that they originate from nominally spin-forbidden dark excitons. Taken together, these observations indicate that dark excitons are funneled to the high-strain regions during their long lifetime and are the principal participants in drift and diffusion at cryogenic temperatures. Our work elucidates the important role that dark excitons play in locally strained WSe$_2$.