Long-lived photoluminescence polarization of localized excitons in liquid exfoliated monolayer enriched WS₂.

Monolayer transition metal dichalcogenides (TMDs) constitute a family of materials, in which coupled spin-valley physics can be explored and which could find applications in novel optoelectronic devices. However, before applications can be designed, a scalable method of monolayer extraction is required. Liquid phase exfoliation is a technique providing large quantities of the monolayer material, but the spin-valley properties of thus obtained TMDs are unknown. In this work, we employ steady-state and time-resolved photoluminescence (PL)to investigate the relaxation dynamics of localized excitons (LXs) in liquid exfoliated WS2. The results reveal that the circular polarization lifetime of the PL exceeds by at least an order of magnitude the PL lifetime. A rate equations model allows us to reproduce quantitatively the experimental data and to conclude that the observed large and long-lived PL polarization originates from efficient trapping of free excitons at localization sites hindering the intervalley relaxation. Furthermore, our results show that the depolarization process is inefficient for LXs. We discuss various mechanisms leading to this effect such as suppression of intervalley scattering of the LXs or inefficient spin relaxation of the holes.