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

ABSTRACT: 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.

SUBMITTER: Chen K

PROVIDER: S-EPMC9900636 | biostudies-literature | 2023 Feb

REPOSITORIES: biostudies-literature

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

Chen K K Luo C C Zhao Y Y Baudelet F F Maurya A A Thamizhavel A A Rößler U K UK Makarov D D Radu F F

The journal of physical chemistry letters 20230124 4

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 fluctua ...[more]

PMID: 36693119

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Project description:Transition-metal chalcogenides with intercalated layered structures are interesting systems in material physics due to their attractive electronic and magnetic properties, with applications in the fields of magnetic refrigerators, catalysts, and thermoelectrics, among others. In this work, we studied in detail the structural, electronic, and magnetic properties of (Fe,Ti)-based sulfides with formula FexTi2S4 (x = 0.24, 0.32, and 0.42), prepared as polycrystalline materials under high-pressure conditions. They present a layered Heideite-type crystal structure, as assessed by synchrotron X-ray diffraction. A local structure analysis using Fe K-edge extended X-ray-absorption fine structure (EXAFS) data unveiled a conspicuous contraction of the main Fe-S bond in Fe0.24Ti2S4 at the vicinity of the magnetic transition 60-80 K. We suggest that this anomaly is related to magnetoelastic coupling effects. The EXAFS analysis allowed extraction of the Einstein temperatures (θE), i.e., the phonon contribution to the specific heat, for the two bond pairs Fe-S(1) [θE ≈318 K; 290 K (C/T)] and Fe-Ti(1) [θE ≈218 K; 190 K (C/T)]. In addition to the structural and local vibrational measurements, we probed the magnetic properties using magneto-calorimetry, magnetometry under applied pressure, magnetoresistance (MR), and Hall effect measurements. We observed the appearance of a broad peak in the specific heat around 120 K in the x = 0.42 compound that we associated with an antiferromagnetic ordering electronic transition. We found that the antiferromagnetic transition temperature is pressure and composition sensitive and reduces at 1.2 GPa by ∼12 and ∼3 K, for the members with x = 0.24 and x = 0.42, respectively. Similarly, the saturation magnetization in the ordered phase depends on both pressure and iron content, reducing its value by 50, 90, and 30% for x = 0.24, 0.32, and 0.42, respectively. We observed clear jumps in the magnetic hysteresis loops, MR, and anomalous Hall effect (AHE) below 2 K at fields around 2-4 T. We associated this observation with the metamagnetic transitions; from the Berry-curvature a decoupling parameter of SH = 0.12 V-1 is determined. Comparison of the results on the temperature-dependent magnetization, MR, and AHE elucidates a strong inelastic scattering contribution to the AHE at higher temperatures due to the cluster spin-glass phase.

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Dataset Information

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

Publications

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

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