Spin-Valley Relaxation of Rydberg Excitons

V. Jindal; K. Mourzidis; M. Semina; D. Lagarde; A. Balocchi; P. Renucci; T. Boulier; T. Taniguchi; K. Watanabe; M. Glazov; X. Marie

arXiv · 2604.07280

Spin-Valley Relaxation of Rydberg Excitons

V. Jindal·K. Mourzidis·M. Semina·D. Lagarde·A. Balocchi·P. Renucci·T. Boulier·T. Taniguchi·K. Watanabe·M. Glazov·X. Marie

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Abstract

Rydberg excitons, characterized by large spatial extension and reduced electron-hole overlap, must have a spin-valley dynamics different from that of ground state excitons. Here we report a direct measurement of spin relaxation of Rydberg excitons in high-quality WSe2 monolayer using continuous-wave and time-resolved optical orientation experiments. Excited excitonic states exhibit exceptionally large photoluminescence circular polarization, approaching 90% for the 3s state. Time-resolved measurements reveal a strong increase of the spin relaxation time with the principal quantum number, from ~2 ps for the 1s exciton to ~75 ps for the 3s exciton. A microscopic model based on electron-hole exchange-driven spin relaxation quantitatively reproduces the observed trend, demonstrating that Rydberg excitons enable tunable spin-valley dynamics in two-dimensional semiconductors.

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V. Jindal, K. Mourzidis, M. Semina, D. Lagarde, A. Balocchi, P. Renucci, T. Boulier, T. Taniguchi, K. Watanabe, M. Glazov, X. Marie. 2026-04-08. Spin-Valley Relaxation of Rydberg Excitons. https://arxiv.org/abs/2604.07280

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