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Register a new userCrystal-field level inversion in lightly Mn-doped Sr3Ru2O7
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Sr3(Ru1-xMnx)2O7, in which 4d-Ru is substituted by the more localized 3d-Mn, is studied by x-ray dichroism and spin-resolved density functional theory. We find that Mn impurities do not exhibit the same 4+ valence of Ru, but act as 3+ acceptors; the extra eg electron occupies the in-plane 3dx2-y2 orbital instead of the expected out-of-plane 3d3z2-r2. We propose that the 3d-4d interplay, via the ligand oxygen orbitals, is responsible for this crystal-field level inversion and the materials transition to an antiferromagnetic, possibly orbitally-ordered, low-temperature state.
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Inelastic neutron scattering (INS), electron spin (ESR) and nuclear magnetic resonance (NMR) measurements were employed to establish the origin of the strong magnetic signal in lightly hole-doped La_{1-x}Sr_xCoO_3, x=0.002. Both, INS and ESR low temperature spectra show intense excitations with large effective g-factors ~10-18. NMR data indicate the creation of extended magnetic clusters. From the Q-dependence of the INS magnetic intensity we conclude that the observed anomalies are caused by the formation of octahedrally shaped spin-state polarons comprising seven Co ions.
We present a temperature-dependent resonant elastic soft x-ray scattering (REXS) study of the metal-insulator transition in Sr3(Ru1-xMnx)2O7, performed at both Ru and Mn L-edges. Resonant magnetic superstructure reflections, which indicate an incipient instability of the parent compound, are detected below the transition. Based on modelling of the REXS intensity from randomly distributed Mn impurities, we establish the inhomogeneous nature of the metal-insulator transition, with an effective percolation threshold corresponding to an anomalously low x<0.05 Mn substitution.
We present a temperature-dependent x-ray absorption (XAS) and resonant elastic x-ray scattering (REXS) study of the metal-insulator transition (MIT) in Sr3(Ru1-xMnx)2O7. The XAS results reveal that the MIT drives the onset of local antiferromagnetic correlations around the Mn impurities, a precursor of the long-range antiferromagnetism detected by REXS at T_order<T_MIT. This establishes that the MIT is of the Mott-type (electronic correlations) as opposed to Slater-type (magnetic order). While this behavior is induced by Mn impurities, the (1/4,1/4,0) order exists for a wide range of Mn concentrations, and points to an inherent instability of the parent compound.
Understanding the nature of charge carriers in doped Mott insulators holds the key to unravelling puzzling properties of strongly correlated electron systems, including cuprate superconductors. Several theoretical models suggested that dopants can be understood as bound states of partons, the analogues of quarks in high-energy physics. However, direct signatures of spinon-chargon bound states are lacking, both in experiment and theory. Here we numerically identify long-lived rotational resonances at low doping, which directly reveal the microscopic structure of spinon-chargon bound states. Similar to Regge trajectories reflecting the quark structure of mesons, we establish a linear dependence of the rotational energy on the super-exchange coupling. Rotational excitations are strongly suppressed in standard angle-resolved photo-emission (ARPES) spectra, but we propose a multi-photon rotational extension of ARPES where they have strong spectral weight. Our findings suggest that multi-photon spectroscopy experiments should provide new insights into emergent universal features of strongly correlated electron systems.
By resonant x-ray scattering at the Mn K-edge on La7/8Sr1/8MnO3, we show that an orbital polaron lattice (OPL) develops at the metal-insulator transition of this compound. This orbital reordering explains consistently the unexpected coexistence of ferromagnetic and insulating properties at low temperatures, the quadrupling of the lattice structure parallel to the MnO2-planes, and the observed polarization and azimuthal dependencies. The OPL is a clear manifestation of strong orbital-hole interactions, which play a crucial role for the colossal magnetoresistance effect and the doped manganites in general.
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