Raman spectroscopy of van der Waals topological magnet GdGaI

Abstract

We report polarization-resolved Raman spectroscopy of a van der Waals compound GdGaI that is a candidate for excitonic insulators. By combining the symmetry analysis with density functional theory calculations, we identify six Raman-active phonons. The spectra exhibit only the expected anharmonic hardening down to 4 K: no additional peaks, no soft modes, and no signatures of zone folding are observed. This result indicates that any lattice distortion is below our experimental sensitivity, supporting an electronically driven origin for the band reconstruction reported by angle-resolved photoemission spectroscopy rather than an electron-phonon-driven mechanism. Moreover, we observe a pronounced circular dichroism of the $A_{1g}$ modes under an out-of-plane magnetic field. Based on symmetry considerations, we attribute this dichroic response to chiral $A_{1g}$ phonons with opposite angular momenta generated by spin-phonon coupling in the time-reversal-broken state. The temperature evolution of the degree of circular polarization further suggests that circularly polarized Raman spectroscopy detects the emergence of short-range antiferromagnetic correlations. Our results highlight GdGaI as a promising platform in which excitonic order, magnetism, and circularly polarized phonons can be intertwined, and demonstrate that circular-polarization Raman provides a sensitive probe of spin-phonon coupling in excitonic systems.