Tuning the Fröhlich exciton-phonon scattering in monolayer MoS2

Abstract: A direct band gap, remarkable light-matter coupling as well as strong spin-orbit and Coulomb interaction establish two-dimensional (2D) crystals of transition metal dichalcogenides (TMDs) as an emerging material class for fundamental studies as well as novel technological concepts. Valley selective optical excitation allows for optoelectronic applications based on the momentum of excitons. In addition to lattice imperfections and disorder, scattering by phonons is a significant mechanism for valley depolarization and decoherence in TMDs at elevated temperatures preventing high-temperature valley polarization required for realistic applications. Thus, a detailed knowledge about strength and nature of the interaction of excitons with phonons is vital. We directly access exciton-phonon coupling in charge tunable single layer MoS2 devices by polarization resolved Raman spectroscopy. We observe a strong defect mediated coupling between the long-range oscillating electric field induced by the longitudinal optical (LO) phonon in the dipolar medium and the exciton. We find that this so-called Fr\"ohlich exciton LO-phonon interaction is suppressed by doping. This suppression correlates with a distinct increase of the degree of valley polarization of up to 20 % even at elevated temperatures of 220 K. Our result demonstrates a promising strategy to increase the degree of valley polarization towards room temperature valleytronic applications.