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Register a new userNature of Well-Screened State in Hard X-ray Mn 2$p$ Core-Level Photoemission of La$_{1-x}$Sr$_x$MnO$_3$ Films
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Using hard x-ray (HX ; $h u$ = 5.95 keV) synchrotron photoemission spectroscopy (PES), we study the intrinsic electronic structure of La$_{1-x}$Sr$_x$MnO$_3$ (LSMO) thin films. Comparison of Mn 2$p$ core-levels with Soft x-ray (SX ; $h u$ $sim$ 1000 eV) -PES shows a clear additional well-screened feature only in HX-PES. Take-off-angle dependent data indicate its bulk ($ge$ 20 {AA}) character. The doping and temperature dependence track the ferromagnetism and metallicity of the LSMO series. Cluster model calculations including charge transfer from doping induced states show good agreement, confirming this picture of bulk properties reflected in Mn 2$p$ core-levels using HX-PES.
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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.
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.
We have investigated change in the electronic structures of atomically-controlled La$_{1-x}$Sr$_x$MnO$_3$ (LSMO) thin films as a function of hole-doping level ($x$) in terms of {it in situ} photoemission spectroscopy (PES) and x-ray absorption spectroscopy (XAS) measurements. The {it in situ} PES measurements on a well-ordered surface of high-quality epitaxial LSMO thin films enable us to reveal their intrinsic electronic structures, especially the structure near the Fermi level ($E_F$). We have found that overall features of valence band as well as the core levels monotonically shifted toward lower binding energy as $x$ was increased, indicating the rigid-band like behavior of underlying electronic structure of LSMO thin films. The peak nearest to $E_F$ due to the $e_g$ orbital is also found to move toward $E_F$ in a rigid-band manner, while the peak intensity decreases with increasing $x$. The loss of spectral weight with $x$ in the occupied density of states was compensated by simultaneous increment of the shoulder structure in O 1$s$ XAS spectra, suggesting the existence of a pseudogap, that is depression in spectral weight at $E_F$, for all metallic compositions. These results indicate that the simple rigid-band model does not describe the electronic structure near $E_F$ of LSMO and that the spectral weight transfer from below to above $E_F$ across the gap dominates the spectral changes with $x$ in LSMO thin films.
To clarify how the electronic state of Sr1-xLaxRuO3 evolves with La doping, we conducted photoemission (PES) experiments using soft x-rays. The spectral shape of the Ru 4d derived peak near the Fermi level changes significantly with increasing x. This variation indicates that a spectral weight transfer from the coherent to incoherent component occurs due to an enhancement of the electron correlation effect. Resonant PES experiments at the La 3d_{5/2} edge have confirmed that there is no significant contribution of the La 5d state in the energy range where the spectral weight transfer is observed. Using the dependence of the photoelectron mean free path on the photon energy, we subtracted the surface components from the PES spectra and confirmed that the enhancement of the electron correlation effect with La doping is an intrinsic bulk phenomenon. On the other hand, a large portion of the coherent component remains at the Fermi level up to x = 0.5, reflecting that the Ru 4d state still has itinerant characteristics. Moreover, we found that the PES spectra hardly depend on the temperature and do not exhibit a discernible change with magnetic ordering, suggesting that the temperature variation of the exchange splitting does not follow the prediction of the Stoner theory. The presently obtained experimental results indicate that the electron correlation effect plays an important role in Sr1-xLaxRuO3 and that the Ru 4d electrons possess both local and itinerant characteristics.
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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