Prolonging Valley Polarization Lifetime through Gate-Controlled Exciton-to-Trion Conversion in Monolayer Molybdenum Ditelluride
arXiv:2111.05560 · doi:10.1038/s41467-022-31672-y
Abstract
Monolayer 2D semiconductors provide an attractive option for valleytronics due to the valley-addressability by helicity-specific light beam. But the short valley lifetime for excitons have hindered potential valleytronic applications. In this paper, we demonstrate a strategy for prolonging the valley lifetime by converting excitons to trions through effective gate control and by taking advantage of much longer valley lifetime for trions than for excitons. In continuous-wave experiments, we found the valley polarization increases as gate voltage is tuned away from the charge neutrality, with the degree of valley polarization increased from near zero to 38 % for excitons and to 33 % for trions. This is the first successful observation of valley-polarization in MoTe2 without a magnetic field. In pump-probe experiments, we found that the intervalley scattering process of excitons is significantly suppressed as gate voltage is tuned away from charge neutrality, with scattering time from 0.85 ps to ~ 2.17 ps. In contrast, the intervalley scattering rate for trions increases due to increased availability of partner charges for trion spin flipping, with scattering time from 1.39 ns down to ~100 ps away from charge neutrality. Interestingly, our results show that, despite the accelerated intervalley scattering, the trion polarization degree increases due to polarized trion generation from the exciton-to-trion conversion overtaking the intervalley trion scatterings. Importantly, the efficient exciton-to-trion conversion changed the dominant depolarization mechanisms. As a result, the valley lifetime is dramatically improved by 1000 times from excitons to trions at the charge neutrality. Our results shed new light into the depolarization dynamics and the interplay of various depolarization channels for excitons and trions and provide an effective strategy for prolonging the valley polarization.
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