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Chiral phonons have been identified in several chiral crystals, primarily in those with trigonal symmetry and threefold screw axes. In this study, chiral phonons in CrSi, a chiral crystal with a sixfold helical structure, were investigated. Circularly polarized Raman spectroscopy revealed a subtle splitting of doubly degenerate phonon modes between cross-circular polarization configurations. These observations, supported by first-principles phonon calculations, indicate the presence of chiral phonons in CrSi, expanding the scope of materials that exhibit chiral vibrational modes beyond the conventional trigonal class.

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