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Doping and bond length contributions to Mn K-edge shift in La$_{1-x}$Sr$_x$MnO$_{3}$ and their correlation with electrical transport properties

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 Added by Ashwani Kumar
 Publication date 2006
  fields Physics
and research's language is English




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The experimental Mn K-edge x-ray absorption spectra of La$_{1-x}$Sr$_x$MnO$_{3}$, $x$ = 0 - 0.7 are compared with the band structure calculations using spin polarized density functional theory. It is explicitly shown that there is a correspondence between the inflection point on the absorption edge and the centre of gravity of the unoccupied Mn 4$p$-band. This correspondence has been used to separate the doping and size contributions to edge shift due to variation in number of electrons in valence band and Mn-O bond lengths, respectively when Sr is doped into LaMnO$_3$. Such separation is helpful to find the localization behaviour of charge carriers and to understand the observed transport properties of these compounds.



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A laboratory hard X-ray photoelectron spectroscopy (HXPS) system equipped with a monochromatic Cr K$alpha$ ($h u = 5414.7$ eV) X-ray source was applied to an investigation of the core-level electronic structure of La$_{1-x}$Sr$_x$MnO$_3$. No appreciable high binding-energy shoulder in the O $1s$ HXPS spectra were observed while an enhanced low binding-energy shoulder structure in the Mn $2p_{3/2}$ HXPS spectra were observed, both of which are manifestation of high bulk sensitivity. Such high bulk sensitivity enabled us to track the Mn $2p_{3/2}$ shoulder structure in the full range of $x$, giving us a new insight into the binding-energy shift of the Mn $2p_{3/2}$ core level. Comparisons with the results using the conventional laboratory XPS ($h u = 1486.6$ eV) as well as those using a synchrotron radiation source ($h u = 7939.9$ eV) demonstrate that HXPS is a powerful and convenient tool to analyze the bulk electronic structure of a host of different compounds.
With x-ray absorption spectroscopy we investigated the orbital reconstruction and the induced ferromagnetic moment of the interfacial Cu atoms in YBa$_2$Cu$_3$O$_{7}$/La$_{2/3}$Ca$_{1/3}$MnO$_3$ (YBCO/LCMO) and La$_{2-x}$Sr$_{x}$CuO$_4$/La$_{2/3}$Ca$_{1/3}$MnO$_3$ (LSCO/LCMO) multilayers. We demonstrate that these electronic and magnetic proximity effects are coupled and are common to these cuprate/manganite multilayers. Moreover, we show that they are closely linked to a specific interface termination with a direct Cu-O-Mn bond. We furthermore show that the intrinsic hole doping of the cuprate layers and the local strain due to the lattice mismatch between the cuprate and manganite layers are not of primary importance. These findings underline the central role of the covalent bonding at the cuprate/manganite interface in defining the spin-electronic properties.
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Due to the complex interplay of magnetic, structural, electronic, and orbital degrees of freedom, biaxial strain is known to play an essential role in the doped manganites. For coherently strained La(2/3)Ca(1/3)MnO(3) thin films grown on SrTiO(3) substrates, we measured the magnetotransport properties both parallel and perpendicular to the substrate and found an anomaly of the electrical transport properties. Whereas metallic behavior is found within the plane of biaxial strain, for transport perpendicular to this plane an insulating behavior and non-linear current-voltage characteristics (IVCs) are observed. The most natural explanation of this anisotropy is a strain induced transition from an orbitally disordered ferromagnetic state to an orbitally ordered state associated with antiferromagnetic stacking of ferromagnetic manganese oxide planes.
The path from a Mott insulating phase to high temperature superconductivity encounters a rich set of unconventional phenomena involving the insulator-to-metal transition (IMT) such as emergent electronic orders and pseudogaps that ultimately affect the condensation of Cooper pairs. A huge hindrance to understanding the origin of these phenomena in the curates is the difficulty in accessing doping levels near the parent state. Recently, the J$_{eff}$=1/2 Mott state of the perovskite strontium iridates has revealed intriguing parallels to the cuprates, with the advantage that it provides unique access to the Mott transition. Here, we exploit this accessibility to study the IMT and the possible nearby electronic orders in the electron-doped bilayer iridate (Sr$_{1-x}$La$_x$)$_3$Ir$_2$O$_7$. Using spectroscopic imaging scanning tunneling microscopy, we image the La dopants in the top as well as the interlayer SrO planes. Surprisingly, we find a disproportionate distribution of La in these layers with the interlayer La being primarily responsible for the IMT, thereby revealing the distinct site-dependent effects of dopants on the electronic properties of bilayer systems. Furthermore, we discover the coexistence of two electronic orders generated by electron doping: a unidirectional electronic order with a concomitant structural distortion; and local resonant states forming a checkerboard-like pattern trapped by La. This provides evidence that multiple charge orders may exist simultaneously in Mott systems, even with only one band crossing the Fermi energy.
We report on Raman scattering measurements of single crystalline La$_{1-x}$Sr$_x$MnO$_3$ ($x$=0, 0.06, 0.09 and 0.125), focusing on the high frequency regime. We observe multi-phonon scattering processes up to fourth-order which show distinct features: (i) anomalies in peak energy and its relative intensity and (ii) a pronounced temperature-, polarization-, and doping-dependence. These features suggest a mixed orbiton-phonon nature of the observed multi-phonon Raman spectra.
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