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Interlayer valley excitons in bilayer MoS2 feature concurrently largeoscillator strength and long lifetime, and hence represent an advantageousscenario for valleytronic applications. However, control of valley pseudospinof interlayer excitons in pristine bilayer MoS2, which lies at the heart ofvalleytronics, has remained elusive. Here we report the observation of highlycircularly polarized photoluminescence from interlayer excitons of bilayer MoS2with both optical and magnetic addressability. Under excitation of circularlypolarized light near exciton resonance, interlayer excitons of bilayer MoS2show a near-unity, but negative circular polarization. Significantly, bybreaking time-reversal symmetry with an out-of-plane magnetic field, a recordlevel of spontaneous valley polarization (7.7%/Tesla) is identified forinterlayer excitons in bilayer MoS2. The giant valley polarization of theinterlayer excitons in bilayer MoS2, together with the feasibility ofelectrical/optical/magnetic control and strong oscillator strength, provides afirm basis for the development of next-generation electronic and optoelectronicapplications.

Optically and magnetically addressable valley pseudospin of interlayer excitons in bilayer MoS2