Raman optical activity (ROA), the dependence of Raman intensity on the circular polarization of incident and scattered light, has traditionally been observed in chiral molecules and magnetic materials, where inversion or time-reversal symmetry is broken. Here we demonstrate that ROA can also arise in a centrosymmetric and nonmagnetic ferroaxial crystal. Using circularly polarized Raman spectroscopy on single-crystalline ${\mathrm{NiTiO}}_3$, we observed a pronounced ROA signal in the cross-circular polarization configurations, which correlates with the ferroaxial domain structure. Our symmetry analysis, first-principles calculations of phonons, and tight-binding model calculations reveal that the natural ROA originates from the ferroaxial order and persists even within the electric dipole approximation. These results establish ROA as a powerful probe of ferroaxial order in centrosymmetric systems.

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• Multipole order
• Optical activity
• Optical phonons
• Density functional theory
• Raman spectroscopy