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Register a new userCompeting electronic instabilities in the quadruple perovskite manganite PbMn$_{7}$O$_{12}$
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Structural behaviour of PbMn$_{7}$O$_{12}$ has been studied by high resolution synchrotron X-ray powder diffraction. This material belongs to a family of quadruple perovskite manganites that exhibit an incommensurate structural modulation associated with an orbital density wave. It has been found that the structural modulation in PbMn$_{7}$O$_{12}$ onsets at 294 K with the incommensurate propagation vector $mathbf{k}_s=(0,0,sim2.08)$. At 110 K another structural transition takes place where the propagation vector suddenly drops down to a emph{quasi}-commensurate value $mathbf{k}_s=(0,0,2.0060(6))$. The emph{quasi}-commensurate phase is stable in the temperature range of 40K - 110 K, and below 40 K the propagation vector jumps back to the incommensurate value $mathbf{k}_s=(0,0,sim2.06)$. Both low temperature structural transitions are strongly first order with large thermal hysteresis. The orbital density wave in the emph{quasi}-commensurate phase has been found to be substantially suppressed in comparison with the incommensurate phases, which naturally explains unusual magnetic behaviour recently reported for this perovskite. Analysis of the refined structural parameters revealed that that the presence of the emph{quasi}-commensurate phase is likely to be associated with a competition between the Pb$^{2+}$ lone electron pair and Mn$^{3+}$ Jahn-Teller instabilities.
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We report a neutron powder diffraction study of $R$Mn$_7$O$_{12}$ quadruple perovskite manganites with $R$ = La, Ce, Nd, Sm, and Eu. We show that in all measured compounds concomitant magnetic ordering of the $A$ and $B$ manganese sublattices occurs on cooling below the N$mathrm{acute{e}}$el temperature. The respective magnetic structures are collinear, with one uncompensated Mn$^{3+}$ moment per formula unit as observed in bulk magnetisation measurements. We show that both LaMn$_7$O$_{12}$ and NdMn$_7$O$_{12}$ undergo a second magnetic phase transition at low temperature, which introduces a canting of the $B$ site sublattice moments that is commensurate in LaMn$_7$O$_{12}$ and incommensurate in NdMn$_7$O$_{12}$. This spin canting is consistent with a magnetic instability originating in the $B$ site orbital order. Furthermore, NdMn$_7$O$_{12}$ displays a third magnetic phase transition at which long range ordering of the Nd sublattice modifies the periodicity of the incommensurate spin canting. Our results demonstrate a rich interplay between transition metal magnetism, orbital order, and the crystal lattice, which may be fine tuned by cation substitution and rare earth magnetism.
By means of synchrotron x-ray and electron diffraction, we studied the structural changes at the charge order transition $T_{CO}$=176 K in the mixed-valence quadruple perovskite (NaMn$_3$)Mn$_4$O$_{12}$. Below $T_{CO}$ we find satellite peaks indicating a commensurate structural modulation with the same propagation vector q =(1/2,0,-1/2) of the CE magnetic order that appears at low temperature, similarly to the case of simple perovskites like La$_{0.5}$Ca$_{0.5}$MnO$_3$. In the present case, the modulated structure together with the observation of a large entropy change at $T_{CO}$ gives evidence of a rare case of full Mn$^{3+}$/Mn$^{4+}$ charge and orbital order consistent with the Goodenough-Kanamori model.
Through a combination of neutron diffraction and Landau theory we describe the spin ordering in the ground state of the quadruple perovskite manganite CaMn7O12 - a magnetic multiferroic supporting an incommensurate orbital density wave that onsets above the magnetic ordering temperature, TN1 = 90 K. The multi-k magnetic structure in the ground state was found to be a nearly-constant-moment helix with modulated spin helicity, which oscillates in phase with the orbital occupancies on the Mn3+ sites via trilinear magneto-orbital coupling. Our phenomenological model also shows that, above TN2 = 48 K, the primary magnetic order parameter is locked into the orbital wave by an admixture of helical and collinear spin density wave structures. Furthermore, our model naturally explains the lack of a sharp dielectric anomaly at TN1 and the unusual temperature dependence of the electrical polarisation.
By means of neutron powder diffraction, we investigated the effect of the polar Bi$^{3+}$ ion on the magnetic ordering of the Mn$^{3+}$ ions in BiMn$_3$Mn$_4$O$_{12}$, the counterpart with textit{quadruple} perovskite structure of the textit{simple} perovskite BiMnO$_3$. The data are consistent with a textit{noncentrosymmetric} spacegroup $Im$ which contrasts the textit{centrosymmetric} one $I2/m$ previously reported for the isovalent and isomorphic compound LaMn$_3$Mn$_4$O$_{12}$, which gives evidence of a Bi$^{3+}$-induced polarization of the lattice. At low temperature, the two Mn$^{3+}$ sublattices of the $A$ and $B$ sites order antiferromagnetically (AFM) in an independent manner at 25 and 55 K, similarly to the case of LaMn$_3$Mn$_4$O$_{12}$. However, both magnetic structures of BiMn$_3$Mn$_4$O$_{12}$ radically differ from those of LaMn$_3$Mn$_4$O$_{12}$. In BiMn$_3$Mn$_4$O$_{12}$ the moments $textbf{M}_{A}$ of the $A$ sites form an anti-body AFM structure, whilst the moments textbf{M}$_{B}$ of the $B$ sites result from a large and textit{uniform} modulation $pm textbf{M}_{B,b}$ along the b-axis of the moments textbf{M}$_{B,ac}$ in the $ac$-plane. The modulation is strikingly correlated with the displacements of the Mn$^{3+}$ ions induced by the Bi$^{3+}$ ions. Our analysis unveils a strong magnetoelastic coupling between the internal strain created by the Bi$^{3+}$ ions and the moment of the Mn$^{3+}$ ions in the $B$ sites. This is ascribed to the high symmetry of the oxygen sites and to the absence of oxygen defects, two characteristics of quadruple perovskites not found in simple ones, which prevent the release of the Bi$^{3+}$-induced strain through distortions or disorder. This demonstrates the possibility of a large magnetoelectric coupling in proper ferroelectrics and suggests a novel concept of internal strain engineering for multiferroics design.
Through analysis of variable temperature neutron powder diffraction data, we present solutions for the magnetic structures of SrMn$_7$O$_{12}$, CdMn$_7$O$_{12}$, and PbMn$_7$O$_{12}$ in all long-range ordered phases. The three compounds were found to have magnetic structures analogous to that reported for CaMn$_7$O$_{12}$. They all feature a higher temperature lock-in phase with emph{commensurate} magneto-orbital coupling, and a delocked, multi-textbf{k} magnetic ground state where emph{incommensurate} magneto-orbital coupling gives rise to a constant-moment magnetic helix with modulated spin helicity. CdMn$_7$O$_{12}$ represents a special case in which the orbital modulation is commensurate with the crystal lattice and involves stacking of fully and partially polarized orbital states. Our results provide a robust confirmation of the phenomenological model for magneto-orbital coupling previously presented for CaMn$_7$O$_{12}$. Furthermore, we show that the model is universal to the $A^{2+}$ quadruple perovskite manganites synthesised to date, and that it is tunable by selection of the $A$-site ionic radius.
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