Spin-Valley Relaxation of Rydberg Excitons

2026/04/08 by V. Jindal, K. Mourzidis, M. Semina +8 · 1 voice
Physics and Astronomy · #cond-mat.other

paper · pdf

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.

Citations

• Interactions of electrons and Rydberg excitons in two-dimensional semiconductors
• Exciton Formation in Two-Dimensional Semiconductors
• Exciton valley depolarization in monolayer transition-metal dichalcogenides
• Intrinsic Lifetime of Higher Excitonic States in Tungsten Diselenide Monolayers
• Revealing exciton masses and dielectric properties of monolayer semiconductors with high magnetic fields
• Luminescent emission of excited Rydberg excitons from monolayer WSe2
• Control of the Exciton Radiative Lifetime in van der Waals Heterostructures
• Exciton States in Monolayer MoSe2 and MoTe2 Probed by Upconversion Spectroscopy
• Exciton-phonon coupling in MoSe2 monolayers
• Exciton Relaxation Cascade in Two-dimensional Transition-metal dichalcogenides
• Superior valley polarization and coherence of 2s excitons in monolayer WSe2
• Optical spectroscopy of excited exciton states in MoS2 monolayers in van der Waals heterostructures
• Magneto-Optics of Exciton Rydberg States in a Monolayer Semiconductor
• Exciton Radiative Lifetime in Transition Metal Dichalcogenide Monolayers
• Magneto-optics in transition metal diselenide monolayers
• Exciton Valley Dynamics probed by Kerr Rotation in WSe2 Monolayers
• Giant Rydberg Excitons in Cuprous Oxide
• Tightly bound excitons in monolayer WSe2
• Non-linear Optical Spectroscopy of Excited Exciton States for Efficient Valley Coherence Generation in WSe2 Monolayers
• Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer WS2
• Exciton fine structure and spin decoherence in monolayers of transition metal dichalcogenides
• Valley dynamics probed through charged and neutral exciton emission in monolayerWSe2
• Bright excitons in monolayer transition metal dichalcogenides: from Dirac cones to Dirac saddle points
• Valley depolarization due to inter- and intra-valley electron-hole exchange interactions in monolayer MoS₂
• Deterministic transfer of two-dimensional materials by all-dry viscoelastic stamping
• Optical Generation of Excitonic Valley Coherence in Monolayer WSe2
• Robust optical emission polarization in MoS2 monolayers through selective valley excitation
• Control of valley polarization in monolayer MoS2 by optical helicity
• Valley-selective circular dichroism of monolayer molybdenum disulphide

Discussions

• V. Jindal, K. Mourzidis, M. Semina, D. Lagarde, A. Balocchi, P. Renucci, T. Boulier, T. Taniguchi, K. Watanabe, M. Glazov, X. Marie: Spin-Valley Relaxation of Rydberg Excitons https://arxiv.org/abs/26 [bsky, 0 points, 0 comments]

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• Magneto-Optics of Exciton Rydberg States in a Monolayer Semiconductor
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