Evidence of the Anomalous Fluctuating Magnetic State by Pressure-Driven 4f Valence Change in EuNiGe 3 .

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 Eu 3+ atomic shell with J = 0, due to intra-atomic exchange and spin-orbital coupling interactions with the Eu 2+ atomic shell. By applying external pressure, a transition from antiferromagnetic to a fluctuating behavior in EuNiGe 3 single crystals is probed. Magnetic polarization is observed for both valence states of Eu 2+ and Eu 3+ 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.