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Register a new userDoping dependence of spin and orbital correlations in layered manganites
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We investigate the interplay between spin and orbital correlations in monolayer and bilayer manganites using an effective spin-orbital t-J model which treats explicitly the e_g orbital degrees of freedom coupled to classical t_{2g} spins. Using finite clusters with periodic boundary conditions, the orbital many-body problem is solved by exact diagonalization, either by optimizing spin configuration at zero temperature, or by using classical Monte-Carlo for the spin subsystem at finite temperature. In undoped two-dimensional clusters, a complementary behavior of orbital and spin correlations is found - the ferromagnetic spin order coexists with alternating orbital order, while the antiferromagnetic spin order, triggered by t_{2g} spin superexchange, coexists with ferro-orbital order. With finite crystal field term, we introduce a realistic model for La_{1-x}Sr_{1+x}MnO_4, describing a gradual change from predominantly out-of-plane 3z^2-r^2 to in-plane x^2-y^2 orbital occupation under increasing doping. The present electronic model is sufficient to explain the stability of the CE phase in monolayer manganites at doping x=0.5, and also yields the C-type antiferromagnetic phase found in Nd_{1-x}Sr_{1+x}MnO_4 at high doping. Also in bilayer manganites magnetic phases and the accompanying orbital order change with increasing doping. Here the model predicts C-AF and G-AF phases at high doping x>0.75, as found experimentally in La_{2-2x}Sr_{1+2x}Mn_2O_7.
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We review our recent x-ray scattering studies of charge and orbital order in doped manganites, with specific emphasis on the role of orbital correlations in Pr_1-xCa_xMnO_3. For x=0.25, we find an orbital structure indistinguishable from the undoped structure with long range orbital order at low temperatures. For dopings 0.3<x<0.5, we find scattering consistent with a charge and orbitally ordered CE-type structure. While in each case the charge order peaks are resolution limited, the orbital order exhibits only short range correlations. We report the doping dependence of the correlation length and discuss the connection between the orbital correlations and the finite magnetic correlation length observed on the Mn^3+ sublattice with neutron scattering techniques. The physical origin of these domains, which appear to be isotropic, remains unclear. We find that weak orbital correlations persist well above the phase transitions, with a correlation length of 1-2 lattice constants at high temperatures. Significantly, we observe similar correlations at high temperatures in La_0.7Ca_0.3MnO_3, which does not have an orbitally ordered ground state, and we conclude that such correlations are robust to variations in the relative strength of the electron-phonon coupling.
Neutron scattering experiments were performed on single crystals of layered cobalt-oxides La2-xCaxCoO4 (LCCO) to characterize the charge and spin orders in a wide hole-doping range of 0.3<x<0.8. For a commensurate value of x=0.5 in (H,0,L) plane, two types of superlattice reflections concomitantly appear at low temperature; one corresponds to a checkerboard charge ordered pattern of Co2+/Co3+ ions and the other is magnetic in origin. Further, the latter magnetic-superlattice peaks show two types of symmetry in the reflections, suggesting antiferromagnetic-stacking (AF-S) and ferromagnetic-stacking (F-S) patterns of spins along the c direction. From the hole-doping dependence, the in-plane correlation lengths of both charge and spin orders are found to give a maximum at x=0.5. These features are the same with those of x=0.5 in La1-xSr1+xMnO4 (LSMO), a typical checkerboard and spin ordered compound. However, in (H,H,L) plane, we found a magnetic scattering peak at Q=(1/4,1/4,1/2) position below TN. This magnetic peak can not be understood by considering the Co2+ spin configuration, suggesting that this peak is originated from Co3+ spin order. By analyzing these superlattice reflections, we found that they are originated from high-spin state of Co3+ spin order.
We study a two-dimensional effective orbital superexchange model derived for strongly correlated e_g electrons coupled to t_{2g} core spins in layered manganites. One finds that the ferromagnetic and antiferromagnetic correlations closely compete, and small changes of parameters can switch the type of magnetic order. For the same reason, spin order is easily destroyed with rising temperature, while alternating orbital correlations can persist to temperatures where FM order has already melted. A scenario for the AF phase observed in LaSrMnO_4 is presented.
We argue that in lightly hole doped perovskite-type Mn oxides the holes (Mn$^{4+}$ sites) are surrounded by nearest neighbor Mn$^{3+}$ sites in which the occupied $3d$ orbitals have their lobes directed towards the central hole (Mn$^{4+}$) site and with spins coupled ferromagnetically to the central spin. This composite object, which can be viewed as a combined orbital-spin-lattice polaron, is accompanied by the breathing type (Mn$^{4+}$) and Jahn-Teller type (Mn$^{3+}$) local lattice distortions. We present calculations which indicate that for certain doping levels these orbital polarons may crystallize into a charge and orbitally ordered ferromagnetic insulating state.
Structural features of the charge/orbital ordering (CO/OO) in single-layered manganites Pr1-xCa1+xMnO4 have been investigated systematically by transmission electron microscopy. Analyses of electron diffraction patterns as well as dark-field images have revealed that the CO/OO shows a striking asymmetric behavior as the hole doping x deviates from x = 0.5. The modulation wavenumber linearly decreases with increasing x in the over-hole-doped (x > 0.5) crystals, while much less dependent on x in the under-hole-doped (x < 0.5) crystals. A temperature-induced incommensurate-commensurate crossover is observed in 0.35 < x < 0.5 and x = 0.65. The correlation length of CO/OO in x = 0.3 was proven to become shorter than that in x > 0.3.
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