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Phonon Chirality Induced by Vibronic-Orbital Coupling

The notion that phonons can carry pseudo-angular momentum has become popular in the last decade, with recent research efforts highlighting phonon chirality, Berry curvature of phonon band structure, and the phonon Hall effect. When a phonon is resonantly coupled to a crystal electric field excitation, a so-called vibronic bound state forms. Here, we observe angular momentum transfer of $δ$Jz = $\pm$1$\hbar$ between phonons and an orbital state in a vibronic bound state of a candidate quantum spin liquid. This observation has profound implications for the engineering of phonon band structure topology through chiral quasiparticle interactions.