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Recently, based on the refined crystal structure of Pr0.6Ca0.4MnO3 from neutron diffraction, Daoud-Aladine et al.[PRL89,97205(2002)] have proposed a new ground state structure for the half-doped manganites R0.5Ca0.5MnO3, where R is a trivalent ion like Bi,La,Pr,Sm or Y. Their proposal describes the CE magnetic structure attributed to these materials as an arrangement of dimers along the ferromagnetic Mn zig-zag chains that form it. However, the dimers proposal is in conflict with the Goodenough-Kanamori-Anderson rules, which give a coherent description of many transition metal insulating compounds and predict the coexistence of Mn3+ and Mn4+ ions in equal parts in the half-doped manganites. On the other hand, Rivadulla et al.[PRB 66, 174432 (2002)] have studied several single crystal samples of half-doped manganites and propose a phase diagram in terms of the tolerance factor which contains both types of structures. In the present work we have calculated the magnon dispersion relations for the CE magnetic structure, arising for each type of proposal: the charge ordered and the dimer phases, respectively. We consider a three-dimensional unit cell containing 16 spins, and compare the magnetic excitations along different paths in the first Brillouin zone. We conclude that measurement of the magnon dispersion relations should allow a clear distinction between the two proposals, predicting qualitative differences arising along specific directions of propagation in the first Brillouin zone.
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Ferromagnetic (FM) manganites, a group of likely half-metallic oxides, are of special interest not only because they are a testing ground of the classical doubleexchange interaction mechanism for the colossal magnetoresistance, but also because they exhibit an extraordinary arena of emergent phenomena. These emergent phenomena are related to the complexity associated with strong interplay between charge, spin, orbital, and lattice. In this review, we focus on the use of inelastic neutron scattering to study the spin dynamics, mainly the magnon excitations in this class of FM metallic materials. In particular, we discussed the unusual magnon softening and damping near the Brillouin zone boundary in relatively narrow band compounds with strong Jahn-Teller lattice distortion and charge/orbital correlations. The anomalous behaviors of magnons in these compounds indicate the likelihood of cooperative excitations involving spin, lattice, as well as orbital degrees of freedom.
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.
We employ time-resolved resonant x-ray diffraction to study the melting of charge order and the associated insulator-metal transition in the doped manganite Pr$_{0.5}$Ca$_{0.5}$MnO$_3$ after resonant excitation of a high-frequency infrared-active lattice mode. We find that the charge order reduces promptly and highly nonlinearly as function of excitation fluence. Density functional theory calculations suggest that direct anharmonic coupling between the excited lattice mode and the electronic structure drive these dynamics, highlighting a new avenue of nonlinear phonon control.
We study the transition at T=0 from a ferromagnetic insulating to a ferromagnetic metallic phase in manganites as a function of hole doping using an effective low-energy model Hamiltonian proposed by us recently. The model incorporates the quantum nature of the dynamic Jahn-Teller(JT) phonons strongly coupled to orbitally degenerate electrons as well as strong Coulomb correlation effects and leads naturally to the coexistence of localized (JT polaronic) and band-like electronic states. We study the insulator-metal transition as a function of doping as well as of the correlation strength U and JT gain in energy E_{JT}, and find, for realistic values of parameters, a ground state phase diagram in agreement with experiments. We also discuss how several other features of manganites as well as differences in behaviour among manganites can be understood in terms of our model.
Phase diagrams in the plane of $r_A$ (the average ionic radius, related to one-electron bandwidth $W$) and $sigma^2$ (the ionic radius variance, measuring the quenched disorder), or ``bandwidth-disorder phase diagrams, have been established for perovskite manganites, with three-dimensional (3$D$) Mn-O network. Here we establish the intrinsic bandwidth-disorder phase diagram of half-doped layered manganites with the two-dimensional (2$D$) Mn-O network, examining in detail the ``mother state of the colossal magnetoresistance (CMR) phenomenon in crystals without ferromagnetic instability. The consequences of the reduced dimensionality, from 3$D$ to 2$D$, on the order-disorder phenomena in the charge-orbital sectors are also highlighted.
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