Efficient valley polarization of charged excitons and resident carriers in MoS2 monolayers by optical pumping

TL;DR

This study demonstrates efficient valley polarization of charged excitons in MoS2 monolayers via optical pumping, revealing large polarization effects and new insights into valley dynamics at cryogenic temperatures.

Contribution

First observation of efficient valley pumping of positively-charged trions in encapsulated MoS2 monolayers, highlighting the role of band structure in valley polarization.

Findings

Negatively-charged trions show 70% polarization.

Large valley polarization achieved with non-resonant excitation.

Circular excitation induces dynamical polarization of resident carriers.

Abstract

We investigate with polarized microphotoluminescence the optical pumping of the valley degree of freedom in charge-tunable MoS2 monolayers encapsulated with hexagonal boron nitride at cryogenic temperatures. We report a large steady state valley polarization of the different excitonic complexes following circularly-polarized laser excitation 25 meV above the neutral exciton transition. For the first time in this material we reveal efficient valley pumping of positively-charged trions, which were so far elusive in non-encapsulated monolayers due to defect and laser-induced large electron doping. We find that negatively-charged trions present a polarization of 70 % which is unusually large for non-resonant excitation. We attribute this large valley polarization to the particular band structure of MoS2, where an optically dark exciton ground state coexists with a bright conduction band ordering in the single-particle picture, leading to a supression of the valley relaxation for negatively-charged trions. In addition, we demonstrate that circular excitation induces a dynamical polarization of resident electrons and holes, as recently shown in tungsten-based monolayers. This manifest itself as a variation in the intensity of different excitonic complexes under circular and linear excitation.