A holistic view of the dynamics of long-lived valley polarized dark excitonic states in monolayer WS2
- Xing Zhu
- David R. Bacon
- Vivek Pareek
- Julien Madéo
- Takashi Taniguchi
- Kenji Watanabe
- Michael K. L. Man
- Keshav M. Dani
2025-07-10
With their long lifetime and protection against decoherence, dark excitons in monolayer semiconductors offer a promising route for quantum technologies. Optical techniques have previously observed dark excitons with a long-lived valley polarization. However, several aspects remain unknown, such as the populations and time evolution of the different valley-polarized dark excitons and the role of excitation conditions. Here, using time- and angle-resolved photoemission spectroscopy, we obtain a holistic view of the dynamics after valley-selective photoexcitation. By varying experimental conditions, we reconcile between the rapid valley depolarization previously reported in TR-ARPES, and the observation of long-lived valley polarized dark excitons in optical studies. For the latter, we find that momentum-dark excitons largely dominate at early times sustaining a 40% degree of valley polarization, while valley-polarized spin-dark states dominate at longer times. Our measurements provide the timescales and how the different dark excitons contribute to the previously observed long-lived valley polarization in optics.