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Register a new userMagnetic order and ice rules in the multiferroic spinel FeV2O4
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We present a neutron diffraction study of FeV2O4, which is rare in exhibiting spin and orbital degrees of freedom on both cation sublattices of the spinel structure. Our data confirm the existence of three structural phase transitions previously identified with x-ray powder diffraction, and reveal that the lower two transitions are associated with sequential collinear and canted ferrimagnetic transitions involving both cation sites. Through consideration of local crystal and spin symmetry, we further conclude that Fe2+ cations are ferro-orbitally ordered below 135K and V3+ orbitals order at 60K in accordance with predictions for vanadium spinels with large trigonal distortions and strong spin-orbit coupling. Intriguingly, the direction of ordered vanadium spins at low temperatures obey `ice rules more commonly associated with the frustrated rare-earth pyrochlore systems.
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We have performed high resolution neutron diffraction and inelastic neutron scattering experiments in the frustrated multiferroic hexagonal compounds RMnO3 (R=Ho, Yb, Sc, Y), which provide evidence of a strong magneto-elastic coupling in the the whole family. We can correlate the atomic positions, the type of magnetic structure and the nature of the spin waves whatever the R ion and temperature. The key parameter is the position of the Mn ions in the unit cell with respect to a critical threshold of 1/3, which determines the sign of the coupling between Mn triangular planes.
Neutron inelastic scattering and diffraction techniques have been used to study the MnV2O4 spinel system. Our measurements show the existence of two transitions to long-range ordered ferrimagnetic states; the first collinear and the second noncollinear. The lower temperature transition, characterized by development of antiferromagnetic components in the basal plane, is accompanied by a tetragonal distortion and the appearance of a gap in the magnetic excitation spectrum. The low-temperature noncollinear magnetic structure has been definitively resolved. Taken together, the crystal and magnetic structures indicate a staggered ordering of the V d orbitals. The anisotropy gap is a consequence of unquenched V orbital angular momentum.
The complex interplay between the 3d and 4f moments in hexagonal ErMnO3 is investigated by magnetization, optical second harmonic generation, and neutron-diffraction measurements. We revise the phase diagram and provide a microscopic model for the emergent spin structures with a special focus on the intermediary phase transitions. Our measurements reveal that the 3d exchange between Mn^{3+} ions dominates the magnetic symmetry at 10 K < T < T_N with Mn^3+ order according to the Gamma_4 representation triggering 4f ordering according to the same representation on the Er^{3+}(4b) site. Below 10 K the magnetic order is governed by 4f exchange interactions of Er^{3+} ions on the 2a site. The magnetic Er^{3+}(2a) order according to the representation Gamma_2 induces a magnetic reorientation (Gamma_4 --> Gamma_2) at the Er^{3+}(4b) and the Mn^{3+} sites. Our findings highlight the fundamentally different roles the Mn^{3+}, R^{3+}(2a), and R^{3+}(4b) magnetism play in establishing the magnetic phase diagram of the hexagonal RMnO3 system.
We have employed resonant x-ray magnetic scattering to specifically probe the magnetic order of the rare-earth ions in multiferroic $mathrm{TbMn_2O_5}$. Two energy resonances were observed, one originated from the E1-E1 dipolar transition and the other from the E2-E2 quadrupolar transition. These resonances directly probe the valence 5d band and the partially occupied 4f band, respectively. First, full polarization analysis, which is a measurement of the scattered polarization as a function of incident polarization, confirmed a spin polarization of the terbium valence states (probed by the E1-E1 transition) by the $mathrm{Mn^{4+}}$ spin density in the commensurate phase. Second, full polarization analysis data were collected in the low-temperature incommensurate and commensurate phases when tuned to the E2-E2 resonance. By employing a least-squares fitting procedure, the spin orientations of the terbium ion sublattice were refined.
By studying the dielectric properties of the geometrically frustrated spinel CdV2O4, we observe ferroelectricity developing at the transition into the collinear antiferromagnetic ground state. In this multiferroic spinel, ferroelectricity is driven by local magnetostriction and not by the more common scenario of spiral magnetism. The experimental findings are corroborated by ab-initio calculations of the electric polarization and the underlying spin and orbital order. The results point towards a charge rearrangement due to dimerization, where electronic correlations and the proximity to the insulator-metal transition play an important role.
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