The moiré superlattice consisting of lattice- or angular-mismatched van der Waals heterostructures drastically changes the physical properties of constituent atomically thin materials by confinement of the exciton by the moiré potential, which is promising for next-generation quantum optics. The moiré superlattice also affects the valley degrees of freedom of the monolayer transition-metal dichalcogenides (TMDs) and the valley-dependent optical selection rule, which results in the characteristic circular polarized light emission of the moiré exciton. However, the valley relaxation process of excitons in the moiré superlattice remains to be understood. Here, we studied valley relaxation of moiré excitons in a twisted WSe2/MoSe2 heterobilayer by circularly polarized photoluminescence and photoluminescence excitation (PLE) spectroscopy. The experimentally observed circularly polarized emission strongly depends on the excitation power density, which contrasts with the case of two-dimensional monolayer TMDs. The excitation power-dependent circularly polarized emission suggests the characteristic valley relaxation of the moiré exciton with a small density of states in zero-dimensional systems. In addition, the resonant PLE measurement reveals the intravalley relaxation process from the triplet to singlet state of the moiré exciton via Γ5 phonon emission. Our findings clarified the valley relaxation of the moiré excitons, which would lead to the application of the circularly polarized quantum light emitter in twisted semiconducting heterobilayers.
Keywords: exciton fine structure; moiré excitons; transition-metal dichalcogenides; van der Waals heterostructures; zero-dimensional system.