Raman Scattering from Higgs Mode Oscillations in the Two-Dimensional Antiferromagnet Ca2RuO4

Abstract

We present and analyze Raman spectra of the Mott insulator Ca2RuO4, whose quasi-two-dimensional antiferromagnetic order has been described as a condensate of low-lying spin-orbit excitons with angular momentum Jeff=1. In the Ag polarization geometry, the amplitude (Higgs) mode of the spin-orbit condensate is directly probed in the scalar channel, thus avoiding infrared-singular magnon contributions. In the B1g geometry, we observe a single-magnon peak as well as two-magnon and two-Higgs excitations. Model calculations using exact diagonalization quantitatively agree with the observations. Together with recent neutron scattering data, our study provides strong evidence for excitonic magnetism in Ca2RuO4 and points out new perspectives for research on the Higgs mode in two dimensions.