We report on the influence of a photochemical doping method on the spin-valley polarization degree (Pc) of excitons in WSe2 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 Pc on the doping level. Using controlled, single-shot photochlorination steps, we unveil this non-monotonic behavior, with Pc 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 5×1011cm−2. The impact of the doping on Pc 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 Pc, 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.
@article{arxiv.2502.03049,
title = {Spin-valley polarization control in WSe$_2$ monolayers using photochemical doping},
author = {E. Katsipoulaki and K. Mourzidis and V. Jindal and D. Lagarde and T. Taniguchi and K. Watanabe and G. Kopidakis and X. Marie and M. M. Glazov and E. Stratakis and G. Kioseoglou and I. Paradisanos},
journal= {arXiv preprint arXiv:2502.03049},
year = {2025}
}