Hidden valley dynamics behind vanishing circular polarization in moiré excitons

Abstract

Optically addressable valley degrees of freedom in transition-metal dichalcogenide heterostructures provide a powerful platform for valleytronic and quantum-optical functionalities. In moiré superlattices, interlayer excitons inherit valley-contrasting optical selection rules while acquiring long lifetimes, electric dipoles, and site-dependent optical responses. However, because conventional measurements typically probe time-integrated valley polarization, the dynamical origin of vanishing polarization has remained elusive. Here, we show that a nearly zero steady-state valley polarization in electrically tunable moiré excitons does not necessarily indicate fast valley relaxation. Helicity-resolved time-resolved photoluminescence reveals a temporal crossing between co- and cross-circularly polarized emission, indicating that helicity-opposite dynamical components coexist and compensate after time integration. A minimal two-channel model, representing A-like and B-like moiré emission channels with opposite optical selection rules and distinct effective decay/depolarization rates, reproduces the observed helicity crossing without invoking a single rapid valley relaxation process. Furthermore, two-dimensional gate-field maps show that the crossing time evolves systematically with electrostatic tuning, demonstrating that the hidden valley dynamics are electrically controllable. These results show that time-integrated circular polarization can give a false-negative indication of valley polarization in multichannel valley emitters.