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Register a new userModulated spin helicity stabilized by incommensurate orbital density waves in a quadruple perovskite manganite
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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.
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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.
Resonant x-ray diffraction experiments were performed for the metallic iridium oxide IrO$_{2}$. We observed anisotropic tensor of susceptibility (ATS) scattering, the spectrum of which shows a sharp contrast between the $L_{3}$ and $L_{2}$ edges. At the $L_{3}$ edge, resonance excitations were clearly observed from the core 2$p$ orbitals to both the 5$d$ $t_{2g}$ and $e_{g}$ orbitals. In contrast, the resonance mode associated with 5$d$ $t_{2g}$ orbitals was indiscernible at the $L_{2}$ edge. This contrasting behavior indicates that Ir 5$d$ $t_{2g}$ orbitals are fairly close to the $J_{rm eff}$ = 1/2 state due to the strong spin--orbit coupling in 5$d$ transition metal ions, as in the Mott insulator Sr$_{2}$IrO$_{4}$. Our results clearly demonstrate that ATS scattering is a useful probe for investigating complex orbital states in a metallic state. Such states induce novel phenomena such as the spin Hall effect.
Both the Jahn-Teller distortion of Cu$^{2+}$O$_6$ octahedra and magnetic ordering are absent in hexagonal Ba$_3$CuSb$_2$O$_9$ suggesting a Cu 3$d$ spin-orbital liquid state. Here, by means of resonant x-ray scattering and absorption experiment, we show that oxygen 2$p$ holes play crucial role in stabilizing this spin-orbital liquid state. These oxygen holes appear due to the reaction Sb$^{5+}$$rightarrow$Sb$^{3+}$ $+$ two oxygen holes, with these holes being able to attach to Cu ions. The hexagonal phase with oxygen 2$p$ holes exhibits also a novel charge-orbital dynamics which is absent in the orthorhombic phase of Ba$_3$CuSb$_2$O$_9$ with Jahn-Teller distortion and Cu 3$d$ orbital order. The present work opens up a new avenue towards spin-charge-orbital entangled liquid state in transition-metal oxides with small or negative charge transfer energy.
Structural study of orbital-ordered manganite thin films has been conducted using synchrotron radiation, and a ground state electronic phase diagram is made. The lattice parameters of four manganite thin films, Nd0.5Sr0.5MnO3 (NSMO) or Pr0.5Sr0.5MnO3 (PSMO) on (011) surfaces of SrTiO3 (STO) or [(LaAlO3){0.3}(SrAl0.5Ta0.5O3){0.7}] (LSAT), were measured as a function of temperature. The result shows, as expected based on previous knowledge of bulk materials, that the films resistivity is closely related to their structures. Observed superlattice reflections indicate that NSMO thin films have an antiferro-orbital-ordered phase as their low-temperature phase while PSMO film on LSAT has a ferro-orbital-ordered phase, and that on STO has no orbital-ordered phase. A metallic ground state was observed only in films having a narrow region of A-site ion radius, while larger ions favor ferro-orbital-ordered structure and smaller ions stabilize antiferro-orbital-ordered structure. The key to the orbital-ordering transition in (011) film is found to be the in-plane displacement along [0-1 1] direction.
The coupling of multiple degrees of freedom - charge, spin, and lattice - in manganites has mostly been considered at the microscopic level. However, on larger length scales, these correlations may be affected by strain and disorder, which can lead to short range order in these phases and affect the coupling between them. To better understand these effects, we explore the dynamics of orbitally ordered domains in a half-doped manganite near the orbital ordering phase transition. Our results suggest that the domains are largely static, and exhibit only slow fluctuations near domain boundaries.
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