Twist angle dependent interlayer transfer of valley polarization from excitons to free charge carriers in WSe$_2$/MoSe$_2$ heterobilayers

TL;DR

This study reveals how twist angle influences valley polarization transfer from excitons to free carriers in WSe₂/MoSe₂ heterobilayers, showing a significant increase in polarization lifetime at larger angles and enabling gate-tunable valley polarization in MoSe₂.

Contribution

It demonstrates twist angle-dependent interlayer scattering mechanisms that enable control over valley polarization transfer and lifetime in heterobilayers, a novel insight for valleytronics.

Findings

Valley polarization transfer efficiency varies with twist angle.

Large twist angles significantly increase valley polarization lifetime.

Gate-tunable valley polarization observed in MoSe₂ due to interlayer transfer.

Abstract

We identify an optical excitation mechanism that transfers a valley polarization from photo-excited electron-hole pairs to free charge carriers in twisted WSe$_2$/MoSe$_2$ heterobilayers. For small twist angles, the valley lifetimes of the charge carriers are surprisingly short, despite the occurrence of interlayer excitons with their presumably long recombination and polarization lifetimes. For large twist angles, we measure an increase in both the valley polarization and its respective lifetime by more than two orders of magnitude. Interestingly, in such heterobilayers we observe an interlayer transfer of valley polarization from the WSe$_2$ layer into the MoSe$_2$ layer. This mechanism enables the creation of a photo-induced valley polarization of free charge carriers in MoSe$_2$, which amplitude scales with the gate-induced charge carrier density. This is in contrast to monolayer MoSe$_2$, where such a gate-tunable valley polarization cannot be achieved. By combining time-resolved Kerr rotation, photoluminesence and angle-resolved photoemission spectroscopy measurements with first principles calculations, we show that these findings can be explained by twist angle dependent interlayer scattering mechanisms involving the Q- and $\Gamma$-valleys.