Unveiling Valley Lifetimes of Free Charge Carriers in Monolayer WSe₂

We report on nanosecond-long, gate-dependent valley lifetimes of free charge carriers in monolayer WSe₂, unambiguously identified by the combination of time-resolved Kerr rotation and electrical transport measurements. While the valley polarization increases when tuning the Fermi level into the conduction or valence band, there is a strong decrease of the respective valley lifetime consistent with both electron-phonon and spin-orbit scattering. The longest lifetimes are seen for spin-polarized bound excitons in the band gap region. We explain our findings via two distinct, Fermi-level-dependent scattering channels of optically excited, valley-polarized bright trions either via dark or bound states. By electrostatic gating we demonstrate that the transition-metal dichalcogenide WSe₂ can be tuned to be either an ideal host for long-lived localized spin states or allow for nanosecond valley lifetimes of free charge carriers (>10 ns).