Understanding Variations in Circularly Polarized Photoluminescence in Monolayer Transition Metal Dichalcogenides

TL;DR

This study investigates the variability in circularly polarized photoluminescence in monolayer transition metal dichalcogenides, revealing an inverse relationship between PL intensity and valley polarization at room temperature.

Contribution

It provides a comprehensive analysis of valley population dynamics in monolayer WS2 and WSe2, highlighting the correlation between sample quality, PL intensity, and polarization.

Findings

Higher PL intensity correlates with lower valley polarization.

Shorter non-radiative lifetimes increase measured polarization.

The observed behavior is consistent across different TMD samples.

Abstract

Monolayer transition metal dichalcogenides are promising materials for valleytronic operations. They exhibit two inequivalent valleys in the Brillouin zone, and the valley populations can be directly controlled and determined using circularly polarized optical excitation and emission. The photoluminescence polarization reflects the ratio of the two valley populations. A wide range of values for the degree of circularly polarized emission, Pcirc, has been reported for monolayer WS2, although the reasons for the disparity are unclear. Here we optically populate one valley, and measure Pcirc to explore the valley population dynamics at room temperature in a large number of monolayer WS2 samples synthesized via chemical vapor deposition. Under resonant excitation, Pcirc ranges from 2% to 32%, and we observe a pronounced inverse relationship between photoluminescence (PL) intensity and Pcirc. High quality samples exhibiting strong PL and long exciton relaxation time exhibit a low degree of valley polarization, and vice versa. This behavior is also demonstrated in monolayer WSe2 samples and transferred WS2, indicating that this correlation may be more generally observed and account for the wide variations reported for Pcirc. Time resolved PL provides insight into the role of radiative and non-radiative contributions to the observed polarization. Short non-radiative lifetimes result in a higher measured polarization by limiting opportunity for depolarizing scattering events.