Coupled ferroelectricity and phonon chirality.

Abstract

Recognizing the coupling between ferroelectricity and chirality in optically active ferroelectrics opens a route for manipulating chirality via ferroelectricity under an external electric field, enabling control over chirality-dependent quantum states. Here, we report the experimental demonstration of the coupling between ferroelectricity and phonon chirality in the molecular ferroelectric triglycine sulfate. By electrically switching the crystal chirality, we achieve reversible and device-compatible control of phonon chirality, as revealed by in situ time-resolved magneto-optical Kerr effect measurements. The Kerr rotation reverses with electric-field switching, while phonon chirality vanishes in the paraelectric phase and is tunable in the racemic ferroelectric state. Furthermore, density functional theory calculations and circularly polarized Raman spectroscopy further corroborate the opposite circular phonon motions. These results establish an electrically addressable coupling pathway linking ferroelectricity, structural chirality, chiral phonons, and spin, opening a route toward chiral-phonon-enabled spin and phonon control technologies based on ferroelectric materials.