Evidence of the Anomalous Fluctuating Magnetic State by Pressure-Driven 4f Valence Change in EuNiGe₃

In rare-earth compounds with valence fluctuation, the proximity of the 4f level to the Fermi energy leads to instabilities of the charge configuration and the magnetic moment. Here, we provide direct experimental evidence for an induced magnetic polarization of the Eu³⁺ atomic shell with J = 0, due to intra-atomic exchange and spin-orbital coupling interactions with the Eu²⁺ atomic shell. By applying external pressure, a transition from antiferromagnetic to a fluctuating behavior in EuNiGe₃ single crystals is probed. Magnetic polarization is observed for both valence states of Eu²⁺ and Eu³⁺ across the entire pressure range. The anomalous magnetism is discussed in terms of a homogeneous intermediate valence state where frustrated Dzyaloshinskii-Moriya couplings are enhanced by the onset of spin-orbital interaction and engender a chiral spin-liquid-like precursor.