Distinct lattice and charge excitations in AV3Sb5 kagome superconductors

The kagome superconductor family A V 3 Sb 5 ( A = Cs, Rb, K) provides a rich platform for exploring diverse electronic symmetry breaking phenomena, including superconductivity and various forms of density wave orders. Although these compounds share the identical lattice structure in the normal state, they exhibit distinct forms of symmetry breaking upon entering the charge density wave (CDW) phase, and the microscopic origin of which remain elusive. Here, we investigate the lattice and charge degrees of freedom in A V 3 Sb 5 using angle-resolved polarized Raman spectroscopy. Our comprehensive polarization-resolved measurements reveal that the lifting of the twofold-degeneracy of the E 2g phonon mode in the CDW phase, previously reported only in CsV 3 Sb 5 with a 3 GHz splitting, also appears ubiquitously in the other two compounds. In contrast, the collective CDW excitations exhibit markedly different polarization dependences depending on the alkali-metal species. These distinct behaviors in the lattice and charge channels provide crucial insight into the enigmatic material-dependent symmetry breaking phenomena that appear in the CDW phase. Furthermore, our experiments, together with first-principles calculations and an effective Hamiltonian model, shed light on the nature of the charge order structure in A V 3 Sb 5 kagome superconductors.