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Journal Articles Physical Review B Year : 2023

Magnetoelastic interactions in SrCu2(BO3)2 studied by Raman scattering experiments and first principles calculations

Abstract

Dynamic and static crystal lattice properties of SrCu2(BO3)2 are studied by means of Raman scattering, magnetostriction, and thermal expansion measurements in magnetic fields to 45 T. Raman experiments versus temperature reveal that some phonon modes show an unusual behavior, their frequencies soften (modes at 200 and 450 cm −1) while others harden (modes at 385 and 478 cm −1) when decreasing the temperature below 15 K. Magneto-Raman experiments show that their field dependence correlates with their respective temperature dependencies, e.g. modes that are hardened with increasing temperature also harden with applied magnetic fields and modes that become softer with temperature also soften with applied fields. We use density functional theory to successfully model and compute the energies of these modes, classifying them in two types: pantograph (modes that when decreasing the temperature) and non-pantograph. We conclude that the former involves the modification of the intra-dimer exchange interaction J and the latter the interdimer J ′. Finally, dilatometry is used to correlate field-dependent Raman modes to the closing of the spin gap as well as fractional-magnetization stripe states M = 1/4 Ms, and M = 1/3 Ms, where Ms is the saturation magnetization.
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Dates and versions

hal-03981318 , version 1 (09-02-2023)

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K. Thirunavukkuarasu, G. Radtke, Z. Lu, M. Lazzeri, P. Christianen, et al.. Magnetoelastic interactions in SrCu2(BO3)2 studied by Raman scattering experiments and first principles calculations. Physical Review B, 2023, 107 (6), pp.064410. ⟨10.1103/PhysRevB.107.064410⟩. ⟨hal-03981318⟩
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