Raman signatures of a non-reciprocal magnetic phase transition in Ca$_2$RuO$_4$

Abstract

The magnetic behavior of Ca$_2$RuO$_4$ represents a unique puzzle due to the interplay of strong electronic correlations, magneto-elastic interactions, and large spin-orbit coupling. At low temperatures, an anomalous Mott insulating state emerges, characterized by a complex antiferromagnetic order with a collective amplitude excitation of the magnetic moment which has been discussed in analogy with the Higgs mode. We report here evidence of a magnetic first-order phase transition driven by an out-of-plane magnetic field along the crystallographic $c$-axis of Ca$_2$RuO$_4$. Raman measurements in magnetic field reveal the emergence of mode of magnetic origin and a concomitant modification of the coupling between a phonon and the Higgs amplitude mode. Both the Raman features are characterized by a non-reciprocal hysteresis in magnetic field. Surprisingly, the observed phase transition does not affect the Raman scattering from the in-plane magnons, indicating that the dipolar antiferromagnetic order is preserved. This is consistent with the onset of a new quadrupolar field-controlled state, whose fluctuations structure can trigger an hybridization between the lattice and the magnetic Higgs mode resulting in the observed Raman features.