<p>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.</p>

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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

摘要

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.