Understanding the Photoluminescence Quenching of Liquid Exfoliated WS2 Monolayers

J Phys Chem C Nanomater Interfaces. 2022 Dec 29;126(51):21681-21688. doi: 10.1021/acs.jpcc.2c05284. Epub 2022 Dec 14.

Abstract

Monolayer transition metal dichalcogenides (TMDs) are being investigated as active materials in optoelectronic devices due to their strong excitonic effects. While mechanical exfoliation (ME) of monolayer TMDs is limited to small areas, these materials can also be exfoliated from their parent layered materials via high-volume liquid phase exfoliation (LPE). However, it is currently considered that LPE-synthesized materials show poor optoelectronic performance compared to ME materials, such as poor photoluminescence quantum efficiencies (PLQEs). Here we evaluate the photophysical properties of monolayer-enriched LPE WS2 dispersions via steady-state and time-resolved optical spectroscopy and benchmark these materials against untreated and chemically treated ME WS2 monolayers. We show that the LPE materials show features of high-quality semiconducting materials such as very small Stokes shift, smaller photoluminescence line widths, and longer exciton lifetimes than ME WS2. We reveal that the energy transfer between the direct-gap monolayers and in-direct gap few-layers in LPE WS2 dispersions is a major reason for their quenched PL. Our results suggest that LPE TMDs are not inherently highly defective and could have a high potential for optoelectronic device applications if improved strategies to purify the LPE materials and reduce aggregation could be implemented.