Observation of ~100% valley-coherent excitons in monolayer MoS2 through giant enhancement of valley coherence time

TL;DR

This paper demonstrates near-perfect valley coherence in monolayer MoS2 excitons by engineering dielectric environment and exciton lifetime, enabling optical readout of valley states.

Contribution

It introduces a novel heterostructure design that achieves fully valley coherent excitons in monolayer MoS2, surpassing previous limitations.

Findings

Achieved ~100% valley coherence in monolayer MoS2 excitons.

Enhanced dielectric screening suppresses exchange interaction.

Reduced exciton lifetime via inter-layer transfer enables motional narrowing.

Abstract

In monolayer transition metal dichalcogenide semiconductors, valley coherence degrades rapidly due to a combination of fast scattering and inter-valley exchange interaction. This leads to a sub-picosecond valley coherence time, making coherent manipulation of exciton a highly challenging task. Using monolayer MoS2 sandwiched between top and bottom graphene, here we demonstrate fully valley coherent excitons by observing ~100% degree of linear polarization in steady state photoluminescence. This is achieved in this unique design through a combined effect of (a) suppression in exchange interaction due to enhanced dielectric screening, (b) reduction in exciton lifetime due to a fast inter-layer transfer to graphene, and (c) operating in the motional narrowing regime. We disentangle the role of the key parameters affecting valley coherence by using a combination of calculation (solutions of Bethe-Salpeter and Maialle-Silva-Sham equations) and a careful choice of design of experiments using four different stacks with systematic variation of screening and exciton lifetime. To the best of our knowledge, this is the first report in which the excitons are found to be valley coherent in the entire lifetime in monolayer semiconductors, allowing optical readout of valley coherence possible.