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Register a new userMagnetic order induced crystal symmetry lowering in ACr$_2$O$_4$ ferrimagnetic spinels
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We demonstrate that the onset of complex spin orders in ACr$_2$O$_4$ spinels with magnetic A$=$Co, Fe and Cu ions lowers the lattice symmetry. This is clearly indicated by the emergence of anisotropic lattice dynamics -- as evidenced by the pronounced phonon splittings -- even when experiments probing static distortions fail. We show that the crystal symmetry in the magnetic phase is reduced from tetragonal to orthorhombic for FeCr$_2$O$_4$ and CuCr$_2$O$_4$ with Jahn-Teller active A-site ions. The conical spin structure in FeCr$_2$O$_4$ is also manifested in the phonon frequencies. In contrast, the multiferroic CoCr$_2$O$_4$ with no orbital degrees of freedom remains nearly cubic in its ground state.
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SrTm$_2$O$_4$ has been investigated using heat capacity, magnetic susceptibility, magnetization in pulsed fields, and inelastic neutron scattering measurements. These results show that the system is highly anisotropic, has gapped low-energy dispersing magnetic excitations, and remains in a paramagnetic state down to 2K. Two theoretical crystal field models were used to describe the single-ion properties of SrTm$_2$O$_4$without any optimization procedures; a standard point-charge model and a Density Functional Theory (DFT) based model that uses Wannier functions. The DFT model was found to better describe the system at low energy by predicting a singlet ground state for one Tm site and a doublet for the second Tm site and anisotropy of second site Tm dominating the anisotropy of the system. Additionally, muon spin rotation/relaxation ($mu^+$psr) spectra reveal oscillations, typically a sign of long-range magnetic order. We attribute these observations to lattice distortion induced by muon implantation, causing renormalization of the gap size.
For a symmetry consistent theoretical description of the multiferroic phase of Ba$_2$CoGe$_2$O$_7$ a precise knowledge of its crystal structure is a prerequisite. In our previous synchrotron X-ray diffraction experiment on multiferroic Ba$_2$CoGe$_2$O$_7$ at room temperature we found forbidden reflections that favour the tetragonal-to-orthorhombic symmetry lowering of the titled compound. Here, we report the results of room-temperature single-crystal diffraction studies with both hot and cold neutrons to differentiate between the real symmetry lowering and multiple diffraction (the Renninger effect). A comparison of the experimental multiple diffraction patterns with simulated ones rules out the symmetry lowering. Thus, the structural model based on the tetragonal space group $Pbar{4}2_1m$ was selected to describe the Ba$_2$CoGe$_2$O$_7$ symmetry at room temperature. The precise structural parameters from neutron diffraction at 300K are presented and compared with the previous X-ray diffraction results.
The magnetism in Mn$_3$Si$_2$Te$_6$ has been investigated using thermodynamic measurements, first principles calculations, neutron diffraction and diffuse neutron scattering on single crystals. These data confirm that Mn$_3$Si$_2$Te$_6$ is a ferrimagnet below a Curie temperature of $T_C$ approximately 78K. The magnetism is anisotropic, with magnetization and neutron diffraction demonstrating that the moments lie within the basal plane of the trigonal structure. The saturation magnetization of approximately 1.6$mu_B$/Mn at 5K originates from the different multiplicities of the two antiferromagnetically-aligned Mn sites. First principles calculations reveal antiferromagnetic exchange for the three nearest Mn-Mn pairs, which leads to a competition between the ferrimagnetic ground state and three other magnetic configurations. The ferrimagnetic state results from the energy associated with the third-nearest neighbor interaction, and thus long-range interactions are essential for the observed behavior. Diffuse magnetic scattering is observed around the 002 Bragg reflection at 120K, which indicates the presence of strong spin correlations well above $T_C$. These are promoted by the competing ground states that result in a relative suppression of $T_C$, and may be associated with a small ferromagnetic component that produces anisotropic magnetism below $approx$330K.
Chiral multiferroic langasites have attracted attention due to their doubly-chiral magnetic ground state within an enantiomorphic crystal. We report on a detailed resonant soft X-ray diffraction study of the multiferroic Ba$_3$TaFe$_3$Si$_2$O$_{14}$ at the Fe $L_{2,3}$ and oxygen $K$ edges. Below $T_N$ ($approx27K$) we observe the satellite reflections $(0,0,tau)$, $(0,0,2tau)$, $(0,0,3tau)$ and $(0,0,1-3tau)$ where $tau approx 0.140 pm 0.001$. The dependence of the scattering intensity on X-ray polarization and azimuthal angle indicate that the odd harmonics are dominated by the out-of-plane ($mathbf{hat{c}}$-axis) magnetic dipole while the $(0,0,2tau)$ originates from the electron density distortions accompanying magnetic order. We observe dissimilar energy dependences of the diffraction intensity of the purely magnetic odd-harmonic satellites at the Fe $L_3$ edge. Utilizing first-principles calculations, we show that this is a consequence of the loss of threefold crystal symmetry in the multiferroic phase.
The very nature of the ground state of the pyrochlore compound Yb$_2$Ti$_2$O$_7$ is much debated, as experimental results demonstrate evidence for both a disordered or a long-range ordered ground state. Indeed, the delicate balance of exchange interactions and anisotropy is believed to lead to competing states, such as a Quantum Spin Liquid state or a ferromagnetic state which may originate from an Anderson-Higgs transition. We present a detailed magnetization study demonstrating a first order ferromagnetic transition at 245 mK and 150 mK in a powder and a single crystal sample respectively. Its first-order character is preserved up to applied fields of $sim$ 200 Oe. The transition stabilizes a ferromagnetic component and involves slow dynamics in the magnetization. Residual fluctuations are also evidenced, the presence of which might explain some of the discrepancies between previously published data for Yb$_2$Ti$_2$O$_7$.
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