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arXiv · 2609.07565

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.

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Giacomo Jarc, Giovanni Tartaglia, Francesco Gabriele, Filomena Forte, Anita Guarino, Angela Montanaro, Enrico Maria Rigoni, Nitesh Khatiwada, Costanza Lincetto, Gabriele Bartolini, Antonio Mastropasqua, Shahla Yasmin Mathengattil, Marco Malvestuto, Muhammad Waqee Ur Rehman, Rosalba Fittipaldi, Joachim Deisenhofer, Alexander A. Tsirlin, Antonio Vecchione, Mario Cuoco, Daniele Fausti. 2026-09-07. Raman signatures of a non-reciprocal magnetic phase transition in Ca$_2$RuO$_4$. https://arxiv.org/abs/2609.07565

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