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Pressure-induced huge increase of Curie temperature of the van der Waals ferromagnet VI3

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 Publication date 2020
  fields Physics
and research's language is English




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Evolution of magnetism in single crystals of the van der Waals compound VI3 in external pressure up to 7.3 GPa studied by measuring magnetization and ac magnetic susceptibility is reported. Four magnetic phase transitions, at T1 = 54.5 K, T2 = 53 K, TC = 49.5 K, and TFM = 26 K, respectively have been observed at ambient pressure. The first two have been attributed to the onset of ferromagnetism in specific crystal-surface layers. The bulk ferromagnetism is characterized by the magnetic ordering transition at Curie temperature TC and the transition between two different ferromagnetic phases TFM, accompanied by a structure transition from monoclinic to triclinic symmetry upon cooling. The pressure effects on magnetic parameters were studied with three independent techniques. TC was found to be almost unaffected by pressures up to 0.6 GPa whereas TFM increases rapidly with increasing pressure and reaches TC at a triple point at ~ 0.85 GPa. At higher pressures, only one magnetic phase transition is observed moving to higher temperatures with increasing pressure to reach 99 K at 7.3 GPa. In contrast, the low-temperature bulk magnetization is dramatically reduced by applying pressure (by more than 50% at 2.5 GPa) suggesting a possible pressure-induced reduction of vanadium magnetic moment. We discussed these results in light of recent theoretical studies to analyze exchange interactions and provide how to increase the Curie temperature of VI3.



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We report structural, physical properties and electronic structure of van der Waals (vdW) crystal VI3. Detailed analysis reveals that VI3 exhibits a structural transition from monoclinic C2/m to rhombohedral R-3 at Ts ~ 79 K, similar to CrX3 (X = Cl, Br, I). Below Ts, a long-range ferromagnetic (FM) transition emerges at Tc ~ 50 K. The local moment of V in VI3 is close to the high-spin state V3+ ion (S = 1). Theoretical calculation suggests that VI3 may be a Mott insulator with the band gap of about 0.84 eV. In addition, VI3 has a relative small interlayer binding energy and can be exfoliated easily down to few layers experimentally. Therefore, VI3 is a candidate of two-dimensional FM semiconductor. It also provides a novel platform to explore 2D magnetism and vdW heterostructures in S = 1 system.
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