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CsYbSe$_2$, a recently identified quantum spin liquid (QSL) candidate,exhibits strong crystal electric field (CEF) excitations. Here, we identifyphonon and CEF modes with Raman spectroscopy and observe strong CEF-phononmixing resulting in a vibronic bound state. Complex, mesoscale interplaybetween phonon modes and CEF modes is observed in real space, and an unexpectednearly resonant condition is satisfied, yielding up to fifth-order combinationmodes, with a total of 17 modes identified in the spectra. This study paves theway to coherent control of possible QSL ground states with optically accessibleCEF-phonon manifolds and mesoscale engineering of CEF-phonon interactions.

Nearly-Resonant Crystalline-Phononic Coupling in Quantum Spin Liquid Candidate CsYbSe$_2$