Raman Scattering from Higgs Mode Oscillations in the Two-Dimensional Antiferromagnet Ca_{2}RuO_{4}

Phys Rev Lett. 2017 Aug 11;119(6):067201. doi: 10.1103/PhysRevLett.119.067201. Epub 2017 Aug 8.

Abstract

We present and analyze Raman spectra of the Mott insulator Ca_{2}RuO_{4}, whose quasi-two-dimensional antiferromagnetic order has been described as a condensate of low-lying spin-orbit excitons with angular momentum J_{eff}=1. In the A_{g} 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 B_{1g} 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 Ca_{2}RuO_{4} and points out new perspectives for research on the Higgs mode in two dimensions.