Magnetic brightening and control of dark excitons in monolayer WSe2

TL;DR

This paper demonstrates how an in-plane magnetic field can turn dark excitons in monolayer WSe2 into bright states, enabling their properties to be experimentally measured and revealing new ways to control optical and valley behaviors.

Contribution

It provides the first direct experimental observation of dark excitons in monolayer WSe2 and shows how magnetic fields can control their optical properties, supported by ab-initio calculations.

Findings

Brightened dark excitons exhibit increased emission and valley lifetimes.

Precise energy levels of dark excitons were measured and matched with theoretical predictions.

Magnetic control offers a new method to tune excitonic and valley properties in 2D semiconductors.

Abstract

Monolayer transition metal dichalcogenide (TMDC) crystals, as direct-gap materials with unusually strong light-matter interaction, have attracted much recent attention. In contrast to the initial understanding, the minima of the conduction band are predicted to be spin split. Because of this splitting and the spin-polarized character of the valence bands, the lowest-lying excitonic states in WX2 (X=S, Se) are expected to be spin-forbidden and optically dark. To date, however, there has been no direct experimental probe of these dark band-edge excitons, which strongly influence the light emission properties of the material. Here we show how an in-plane magnetic field can brighten the dark excitonic states and allow their properties to be revealed experimentally in monolayer WSe2. In particular, precise energy levels for both the neutral and charged dark excitons were obtained and compared with ab-initio calculations using the GW-BSE approach. Greatly increased emission and valley lifetimes were observed for the brightened dark states as a result of their spin configuration. These studies directly probe the excitonic spin manifold and provide a new route to tune the optical and valley properties of these prototypical two-dimensional semiconductors.