Magneto-optic phonon resonances in magnetic topological EuCd2As2 via helical Raman spectroscopy

Abstract

EuCd2As2 materials have two magnetic ordering states: antiferromagnetic (AFM) and ferromagnetic (FM) when their chemical tunability is utilized. While AFM-EuCd2As2 has a nonzero magnetoelectric response due to its symmetry breaking with spin configuration, FM-EuCd2As2 is an ideal candidate for studies of Weyl physics because of its minimum number of Weyl points with opposite chirality. In this article, we examine cryogenic low-frequency Raman spectroscopy of phonon modes in FM-EuCd2As2 crystals using circular polarization configurations, with support from density functional theory calculations, and investigate in-plane magneto-anisotropy by linear polarization configuration below the Curie temperature (Tc = 26 K). We attribute the anomalous enhancements in Raman intensities below the Curie temperature are due to spin-phonon coupling. Furthermore, we see that A-mode peaks can be distinguished by magneto-helical Raman spectroscopy through the magneto-optic effect and that the degree of circular polarization (DCP) of 12.5 meV peak reaches 60% at 4.2 K and becomes saturated. We also examine AFM-EuCd2As2 below Néel temperature (TN = 9 K) to compare with FM-EuCd2As2, but we hardly observe spin-phonon coupling and find negligible DCP values due to almost zero net magnetization. Our results contribute to the understanding of the phonon dynamics and the interplay between topology and magnetism in FM-EuCd2As2, through helical light and external magnetic fields. This lays the foundation for utilizing state-of-the-art Weyl systems for applications in thermoelectrics, phononic devices, and topological quantum computing.