Spin-valley polarization control in WSe$_2$ monolayers using photochemical doping

TL;DR

This study demonstrates how photochemical doping can modulate spin-valley polarization in WSe$_2$ monolayers, revealing a non-monotonic dependence on carrier density and identifying exciton-carrier interactions as key factors.

Contribution

It introduces a controlled photochemical doping technique to tune and analyze spin-valley polarization in WSe$_2$ monolayers, providing new insights into exciton dynamics.

Findings

Non-monotonic polarization dependence on doping level

Maximum polarization increase by a factor of three at specific hole density

Exciton-carrier collisions dominate polarization variations

Abstract

We report on the influence of a photochemical doping method on the spin-valley polarization degree ($P_{c}$) of excitons in WSe$_2$ monolayers. By varying the carrier density and transitioning from an excess of electrons (n-type) to an excess of holes (p-type), we observe a non-monotonic dependence of $P_{c}$ on the doping level. Using controlled, single-shot photochlorination steps, we unveil this non-monotonic behavior, with $P_{c}$ reaching a minimum value of less than 10$\%$ at 78 K near the charge neutrality point, while increasing by a factor of three at a hole density of $5 \times 10^{11} \,\mathrm{cm^{-2}}$. The impact of the doping on $P_{c}$ is explained using a phenomenological model that accounts for various mechanisms influencing exciton polarization dynamics, including exciton-carrier scattering processes and exciton-to-trion conversion rates. Among these, exciton-carrier collisions emerge as the dominant mechanism driving the observed variations in $P_{c}$, while the exciton effective lifetime remains nearly independent of doping. These findings highlight the potential of photochemical methods for investigating valley physics and for effectively tuning the exciton polarization degree in transition metal dichalcogenide monolayers.