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Register a new userHexagonal phase stabilization and magnetic orders of multiferroic Lu$_{1-x}$Sc$_x$FeO$_3$
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Hexagonal LuFeO$_3$ has drawn a lot of research attention due to its contentious room-temperature multiferroicity. Due to the unstability of hexagonal phase in the bulk form, most experimental studies focused on LuFeO$_3$ thin films which can be stabilized by strain using proper substrates. Here we report on the hexagonal phase stabilization, magnetism, and magnetoelectric coupling of bulk LuFeO$_3$ by partial Sc-substitution of Lu. First, our first-principles calculations show that the hexagonal structure can be stabilized by partial Sc substitution, while the multiferroic properties including the noncollinear magnetic order and geometric ferroelectricity remain robustly unaffected. Therefore, Lu$_{1-x}$Sc$_x$FeO$_3$ can act as a platform to check the multiferroicity of LuFeO$_3$ and related materials in the bulk form. Second, the magnetic characterizations on bulk Lu$_{1-x}$Sc$_x$FeO$_3$ demonstrate a magnetic anomaly (probable antiferromagnetic ordering) above room temperature, $sim425-445$ K, followed by magnetic transitions in low temperatures ($sim167-172$ K). In addition, a magnetoelectric response is observed in the low temperature region. Our study provides useful information on the multiferroic physics of hexagonal $R$FeO$_3$ and related systems.
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Non-collinear two-dimensional triangular lattice antiferromagnets (2D TLAF) are currently an area of very active research due to their unique magnetic properties, which lead to non-trivial quantum effects that experimentally manifest themselves in the spin excitation spectra. Recent examples of such insulating 2D TLAF include (Y,Lu)MnO$_3$, LiCrO$_2$, and CuCrO$_2$. Hexagonal LuFeO3 is a recently synthesized 2D TLAF which exhibits properties of an ideal multiferroic material, partially because of the high spin ($S=5/2$) and strong magnetic super-exchange interactions. We report the full range of spin dynamics in a bulk single crystal of (Lu$_{0.6}$Sc$_{0.4}$)FeO$_3$ (Sc doping to stabilize the hexagonal structure) measured via time-of-flight inelastic neutron scattering. Modeling with linear spin wave theory yields a nearest neighbor exchange coupling of $J$ = 4.0(2) meV (DFT calculations for $h$-LuFeO$_3$ predicted a value of 6.31 meV) and anisotropy values of $K_D$ = 0.17(1) meV (easy plane) and $K_A$~=~-0.05(1)~meV (local easy axis). It is observed that the magnon bandwidth of the spin wave spectra is twice as large for $h$-(Lu,Sc)FeO$_3$ as it is for $h$-LuMnO$_3$.
For disordered Heisenberg systems with small single ion anisotropy, two spin glass transitions below the long range ordered phase transition temperature has been predicted theoretically for compositions close to the percolation threshold. Experimental verification of these predictions is still controversial for conventional spin glasses. We show that multiferroic spin glass systems can provide a unique platform for verifying these theoretical predictions via a study of change in magnetoelastic and magnetoelectric couplings, obtained from an analysis of diffraction data, at the spin glass transition temperatures. Results of macroscopic and microscopic (x-ray and neutron scattering) measurements are presented on disordered BiFeO3, a canonical Heisenberg system with small single ion anisotropy, which reveal appearance of two spin glass phases SG1 and SG2 in coexistence with the LRO phase below the A-T and G-T lines. It is shown that the temperature dependence of the integrated intensity of the antiferromagnetic peak shows dips with respect to the Brillouin function behaviour around the SG1 and SG2 transition temperatures. The ferroelectric polarisation changes significantly at the two spin glass transition temperatures. These results, obtained using microscopic techniques, clearly demonstrate that the SG1 and SG2 transitions occur on the same magnetic sublattice and are intrinsic to the system. We also construct a phase diagram showing all the magnetic phases in BF-xBT system. While our results on the two spin glass transitions support the theoretical predictions, it also raises several open questions which need to be addressed by revisiting the existing theories of spin glass transitions by taking into account the effect of magnetoelastic and magnetoelectric couplings as well as electromagnons.
We present a theoretical analysis of the magnetic phase diagram of CeTi$_{1-x}$Sc$_{x}$Ge and GdFe$_{1-x}$Co$_{x}$Si as a function of the temperature and the Sc and Co concentration $x$, respectively. CeScGe and GdCoSi, as many other RTX (R=rare earth, T=transition metal, X=p-block element) compounds, present a tetragonal crystal structure where bilayers of R are separated by layers of T and X. While GdFeSi and CeTi$_{0.75}$Sc$_{0.25}$Ge are ferromagnetic, CeScGe and GdCoSi order antiferromagnetically with the R 4f magnetic moments on the same bilayer aligned ferromagnetically and magnetic moments in nearest neighbouring bilayers aligned antiferromagnetically. The antiferromagnetic transition temperature $T_N$ decreases with decreasing concentration $x$ in both compounds and for low enough values of $x$ the compounds show a ferromagnetic behavior. Based on these observations we construct a simplified model Hamiltonian that we solve numerically for the specific heat and the magnetization. We find a good qualitative agreement between the model and the experimental data. Our results show that the main magnetic effect of the Sc $to$ Ti and Co $to$ Fe substitution in these compounds is consistent with a change in the sign of the exchange coupling between magnetic moments in neighbouring bilayers. We expect a similar phenomenology for other magnetic RTX compounds with the same type of crystal structure.
A detailed electronic phase diagram of perovskite-type oxides Sr$_{1-x}$La$_x$FeO$_3$ $(0leq x leq 0.5)$ was established by synchrotron X-ray diffraction, magnetization, and transport measurements for polycrystalline samples synthesized by a high-pressure technique. Among three kinds of helimagnetic phases in SrFeO$_3$ at zero field, two of them showing multiple-${it q}$ helimagnetic spin textures tend to rapidly disappear in cubic symmetry upon the La substitution with $x$ less than 0.1, which accompanies the loss of metallic nature. On the other hand, the third helimagnetic phase apparently remains robustly in Sr$_{1-x}$La$_x$FeO$_3$ with $x$ higher than 0.1, followed by merging to the spin/charge ordered phase with $xsim 1/3$. We propose an important role of itinerant ligand holes on the emergence of multiple-${it q}$ states and a possible link between the third (putative single-${it q}$) helimagnetic phase in SrFeO$_3$ and the spin/charge ordered phase in Sr$_{2/3}$La$_{1/3}$FeO$_3$.
Hexagonal rare-earth ferrite RFeO$_3$ family represents a unique class of multiferroics exhibiting weak ferromagnetism, and a strong coupling between magnetism and structural trimerization is predicted. However, the hexagonal structure for RFeO$_3$ remains metastable in conventional condition. We have succeeded in stabilizing the hexagonal structure of polycrystalline YbFeO$_3$ by partial Sc substitution of Yb. Using bulk magnetometry and neutron diffraction, we find that Yb$_{0.42}$Sc$_{0.58}$FeO$_3$ orders into a canted antiferromagnetic state with the Neel temperature $T_N$ ~ 165 K, below which the $Fe^{3+}$ moments form the triangular configuration in the $ab$-plane and their in-plane projections are parallel to the [100] axis, consistent with magnetic space group $P$6$_{3}$$cm$. It is determined that the spin-canting is aligned along the $c$-axis, giving rise to the weak ferromagnetism. Furthermore, the $Fe^{3+}$ moments reorient toward a new direction below reorientation temperature $T_R$ ~ 40 K, satisfying magnetic subgroup $P$6$_{3}$, while the $Yb^{3+}$ moments order independently and ferrimagnetically along the $c$-axis at the characteristic temperature $T_{Yb}$ ~ 15 K. Interestingly, reproducible modulation of electric polarization induced by magnetic field at low temperature is achieved, suggesting that the delicate structural distortion associated with two-up/one-down buckling of the Yb/Sc-planes and tilting of the FeO$_5$ bipyramids may mediate the coupling between ferroelectric and magnetic orders under magnetic field. The present work represents a substantial progress to search for high-temperature multiferroics in hexagonal ferrites and related materials.
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