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Register a new userOrbital order in La0.5Sr1.5MnO4: beyond a common local Jahn-Teller picture
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The standard way to find the orbital occupation of Jahn-Teller (JT) ions is to use structural data, with the assumption of a one-to-one correspondence between the orbital occupation and the associated JT distortion, e.g. in O6 octahedron. We show, however, that this approach in principle does not work for layered systems. Specifically, using the layered manganite La0.5Sr1.5MnO4 as an example, we found from our x-ray absorption measurements and theoretical calculations, that the type of orbital ordering strongly contradicts the standard local distortion approach for the Mn3+O6 octahedra, and that the generally ignored long-range crystal field effect and anisotropic hopping integrals are actually crucial to determine the orbital occupation. Our findings may open a pathway to control of the orbital state in multilayer systems and thus of their physical properties.
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The origin of the cooperative Jahn-Teller distortion and orbital-order in LaMnO3 is central to the physics of the manganites. The question is complicated by the simultaneous presence of tetragonal and GdFeO3-type distortions and the strong Hunds rule coupling between e_g and t_2g electrons. To clarify the situation we calculate the transition temperature for the Kugel-Khomskii superexchange mechanism by using the local density approximation+dynamical mean-field method, and disentangle the effects of super-exchange from those of lattice distortions. We find that super-exchange alone would yield T_KK=650 K. The tetragonal and GdFeO3-type distortions, however, reduce T_KK to 550 K. Thus electron-phonon coupling is essential to explain the persistence of local Jahn-Teller distortions to at least 1150 K and to reproduce the occupied orbital deduced from neutron scattering.
We consider the superexchange in `frustrated Jahn-Teller systems, such as the transition metal oxides NaNiO_2, LiNiO_2, and ZnMn_2O_4, in which transition metal ions with doubly degenerate orbitals form a triangular or pyrochlore lattice and are connected by the 90-degree metal-oxygen-metal bonds. We show that this interaction is much different from a more familiar exchange in systems with the 180-degree bonds, e.g. perovskites. In contrast to the strong interplay between the orbital and spin degrees of freedom in perovskites, in the 90-degree exchange systems spins and orbitals are decoupled: the spin exchange is much weaker than the orbital one and it is ferromagnetic for all orbital states. Due to frustration, the mean-field orbital ground state is strongly degenerate. Quantum orbital fluctuations select particular ferro-orbital states, such as the one observed in NaNiO_2. We also discuss why LiNiO_2 may still behave as an orbital liquid.
Using high resolution X-Ray diffraction (XRD) on high purity powders, we resolved the structure and $ab$ symmetry of the intriguing compound svo$ $ from room temperature down to 20 K to an unprecedented level of accuracy. Upon cooling, this new set of data unambiguously reveals a second order phase transition lowering the symmetry from tetragonal to orthorhombic at a temperature $T_{c2}=136$ K. The observation of an orthorhombic distortion of the $ab$-plane is attributed to nematic phase formation supported by local Jahn-Teller (JT) dynamical instability. At $T_{N}=105$ K, spins order and at $T_{c1}=100$ K the tetragonal structure is recovered with an elongated c-axis.
We report on combined neutron and resonant x-ray scattering results, identifying the nature of the spin-orbital ground state and magnetic excitations in LuVO3 as driven by the orbital parameter. In particular, we distinguish between models based on orbital Peierls dimerization, taken as a signature of quantum effects in orbitals, and Jahn-Teller distortions, in favor of the latter. In order to solve this long-standing puzzle, polarized neutron beams were employed as a prerequisite in order to solve details of the magnetic structure, which allowed quantitative intensity-analysis of extended magnetic excitation data sets. The results of this detailed study enabled us to draw definite conclusions about classical vs quantum behavior of orbitals in this system and to discard the previous claims about quantum effects dominating the orbital physics of LuVO3 and similar systems.
In-plane anisotropic ground states are ubiquitous in correlated solids such as pnictides, cuprates and manganites. They can arise from doping Mott insulators and compete with phases such as superconductivity, however their origins are debated. Strong coupling between lattice, charge, orbital and spin degrees of freedom results in simultaneous ordering of multiple parameters, masking the mechanism that drives the transition. We demonstrate that the anisotropic orbital domains in a manganite can be oriented by the polarization of a pulsed THz light field. Through the application of the Hubbard model, we show that domain control can be achieved either through field assisted hopping of charges or a field-induced modification of bond angles. Both routes enhance the local Coulomb repulsions which drive domain reorientation and the dominant mechanism is dictated by the equilibrium Mn-O-Mn bond angle. Our results highlight the key role played by the Coulomb interaction in driving orbital order in manganites and demonstrate how THz can be utilized in new ways to understand and manipulate anisotropic phases in a broad range of correlated materials.
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