The Chirality of Phonons: Definitions, Symmetry Constraints, and Experimental Observation

Abstract: Circularly polarized phonons with nonzero angular momentum (AM), also referred to as chiral phonons, have garnered increasing attention in recent studies. Many existing experimental/theoretical works identify chiral phonons based on pseudo-angular momentum (PAM) or the flipping of the polarization of the circularly polarized light (CPL) in the Raman scattering process. However, the accuracy and universality of these assumptions remain to be verified. Moreover, in condensed matter physics, symmetry strongly governs the scattering and interactions of phonons, quasi-particles, and external fields, profoundly affecting correlated physical phenomena. In this study, we first conduct an in-depth examination of the distinctions and interconnections among AM, PAM, helicity, and atomic motion--key characteristics inherent to chiral phonons--and then undertake a comprehensive study of phonon chirality, as well as their associated physical quantities, and experimental benchmarks under various magnetic point groups. By developing the symmetry-based framework for phonon chirality across magnetic point groups, we demonstrate that identifying chiral phonons solely through nonzero PAM or CPL polarization inversion is inadequate, challenging prior findings. This framework clarifies the relationship between symmetry and phonon chirality, revealing that phonon modes governed by different symmetries exhibit distinct experimental signatures, thereby advancing our understanding of these phenomena. Finally, experiments on five materials with distinct symmetries are conducted to validate our theoretical results. Supported by both theoretical rigor and experimental validation, our study represents a significant step forward in advancing research on symmetry-constrained phonons.