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Opletal, P.
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article
Pressure-induced large increase of Curie temperature of the van der Waals ferromagnet VI3
Abstract
Evolution of magnetism in single crystals of the van der Waals compound VI<sub>3</sub> in external pressure up to 7.3 GPa studied by measuring magnetization and ac magnetic susceptibility is reported. Four magnetic phase transitions, at T<sub>1</sub>=54.5K, T<sub>2</sub>=53K, T<sub>C</sub>=49.5K, and T<sub>FM</sub>=26K, 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 T<sub>C</sub> and the transition between two different ferromagnetic phases T<sub>FM</sub>, accompanied by a structure transition from monoclinic to triclinic symmetry upon cooling. The pressure effects on magnetic parameters were studied with three independent techniques. T<sub>C</sub> was found to be almost unaffected by pressures up to 0.6 GPa whereas T<sub>FM</sub> increases rapidly with increasing pressure and reaches T<sub>C</sub> 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 significantly reduced by applying pressure (by more than 50% at 2.5 GPa) suggesting a possible pressure-induced reduction of vanadium magnetic moment. First-principles calculations of VI<sub>3</sub> under pressure allow us to ascribe the evolution of T<sub>C</sub> with pressure to the reduction of interplanar distance, including the observed slope change at 0.6 GPa. These calculations also describe the associated band gap closing, showing that with a modest compression the material would become metallic. Overall, the large pressure range covered corresponds to a significant change of interplanar interactions. The obtained data thus allow us to shed light on how does the transition between the three-dimensional (3D) and quasi-2D system affect magnetic interactions in the system.