Persistent room-temperature valley polarization in graphite-filtered WS2 monolayer

Abstract

Transition metal dichalcogenide (TMD) monolayers (1L) in the 2H-phase are two-dimensional semiconductors with two valleys in their band structure that can be selectively populated using circularly polarized light. The choice of the substrate for monolayer TMDs is an essential factor for the optoelectronic properties and for achieving a high degree of valley polarization at room temperature (RT). In this work, we investigate the RT valley polarization of monolayer WS2 on different substrates. A degree of polarization of photoluminescence (PL) in excess of 27% is found from neutral excitons in 1L-WS2 on graphite at RT, under resonant excitation. Using chemical doping through photochlorination we modulate the polarization of the neutral exciton emission from 27% to 38% for 1L-WS2/graphite. We show that the valley polarization strongly depends on the interplay between doping and the choice of the supporting layer of TMDs. Time-resolved PL measurements, corroborated by a rate equation model accounting for the bright exciton population in the presence of a dark exciton reservoir support our findings. These results suggest a pathway towards engineering valley polarization and exciton lifetimes in TMDs, by controlling the carrier density and/or the dielectric environment at ambient conditions.