Ultrafast dynamics of coherent exciton-polaritons in van der Waals semiconductor metasurfaces

Abstract

Enabling coherent light-matter interactions is a critical step toward next-generation quantum technologies. However, achieving this under ambient temperature conditions remains challenging due to rapid dephasing in optically excited systems. Optical metasurfaces based on quasi-bound states in the continuum have recently emerged as a powerful platform for reaching the strong light-matter coupling regime in flat, subwavelength thickness devices. Here, we investigate ultrafast exciton-polariton dynamics in self-hybridized WS${}_2$ thin-film metasurfaces. Using hyperspectral momentum-resolved imaging, we reconstruct the highly anisotropic exciton-polariton dispersion, with a transition from positive to negative effective mass along orthogonal symmetry axes. Femtosecond pump-probe and multidimensional spectroscopy reveal detuning-dependent polariton dynamics with a coherence time up to ~110 fs, and allow direct observation of the coherent dynamics through ultrafast Rabi oscillations with ~45 fs period. We describe this behaviour with a three-eigenstate model that couples the photonic resonance with both bright and dark excitons, extending the conventional two-state picture of strong coupling. Our results establish van der Waals metasurfaces as a promising platform for next-generation polaritonic devices, enabling coherent quantum transfer of matter excitations at room temperature.

14 pages, 4 main figures