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Register a new userThe electronic structure of epitaxially stabilized 5d perovskite Ca_{1-x}Sr_xIrO_3 (x = 0, 0.5, and 1) thin films: the role of strong spin-orbit coupling
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We have investigated the electronic structure of meta-stable perovskite Ca1-xSrxIrO3 (x = 0, 0.5, and 1) thin films using transport measurements, optical spectroscopy, and first-principles calculations. We artificially fabricated the perovskite phase of Ca1-xSrxIrO3, which has a hexagonal or post perovskite crystal structure in bulk form, by growing epitaxial thin films on perovskite GdScO3 substrates using epi-stabilization technique. The transport properties of the perovskite Ca1-xSrxIrO3 films systematically changed from nearly insulating (or semi-metallic) for x = 0 to bad metallic for x = 1. Due to the extended wavefunctions, 5d electrons are usually delocalized. However, the strong spin-orbit coupling in Ca1-xSrxIrO3 results in the formation of effective total angular momentum Jeff = 1/2 and 3/2 states, which puts Ca1-xSrxIrO3 in the vicinity of a metal-insulator phase boundary. As a result, the electrical properties of the Ca1-xSrxIrO3 films are found to be sensitive to x and strain.
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We have studied the electronic structure of Li$_{1+x}$[Mn$_{0.5}$Ni$_{0.5}$]$_{1-x}$O$_2$ ($x$ = 0.00 and 0.05), one of the promising cathode materials for Li ion battery, by means of x-ray photoemission and absorption spectroscopy. The results show that the valences of Mn and Ni are basically 4+ and 2+, respectively. However, the Mn$^{3+}$ component in the $x$ = 0.00 sample gradually increases with the bulk sensitivity of the experiment, indicating that the Jahn-Teller active Mn$^{3+}$ ions are introduced in the bulk due to the site exchange between Li and Ni. The Mn$^{3+}$ component gets negligibly small in the $x$ = 0.05 sample, which indicates that the excess Li suppresses the site exchange and removes the Jahn-Teller active Mn$^{3+}$.
Single crystals of the perovskite-type $3d^{1}$ metallic alloy system Ca$_{1-x}$Sr$_x$VO$_3$ were synthesized in order to investigate metallic properties near the Mott transition. The substitution of a Ca$^{2+}$ ion for a Sr$^{2+}$ ion reduces the band width $W$ due to a buckling of the V-O-V bond angle from $sim180^circ$ for SrVO$_3$ to $sim160^circ$ for CaVO$_3$. Thus, the value of $W$ can be systematically controlled without changing the number of electrons making Ca$_{1-x}$Sr$_x$VO$_3$: one of the most ideal systems for studying band-width effects. The Sommerfeld-Wilsons ratio ($simeq2$), the Kadowaki-Woods ratio (in the same region as heavy Fermion systems), and a large $T^{2}$ term in the electric resistivity, even at 300 K, substantiate a large electron correlation in this system, though the effective mass, obtained by thermodynamic and magnetic measurements, shows only a systematic but moderate increase in going from SrVO$_3$ to CaVO$_3$, in contrast to the critical enhancement expected from the Brinkmann-Rice picture. It is proposed that the metallic properties observed in this system near the Mott transition can be explained by considering the effect of a non-local electron correlation.
We present the electronic structure of Sr_{1-(x+y)}La_{x+y}Ti_{1-x}Cr_{x}O_{3} investigated by high-resolution photoemission spectroscopy. In the vicinity of Fermi level, it was found that the electronic structure were composed of a Cr 3d local state with the t_{2g}^{3} configuration and a Ti 3d itinerant state. The energy levels of these Cr and Ti 3d states are well interpreted by the difference of the charge-transfer energy of both ions. The spectral weight of the Cr 3d state is completely proportional to the spin concentration x irrespective of the carrier concentration y, indicating that the spin density can be controlled by x as desired. In contrast, the spectral weight of the Ti 3d state is not proportional to y, depending on the amount of Cr doping.
We investigate the electronic structure of the metallic NiS$_{1-x}$Se$_x$ system using various electron spectroscopic techniques. The band structure results do not describe the details of the spectral features in the experimental spectrum, even for this paramagnetic metallic phase. However, a parameterized many-body multi-band model is found to be successful in describing the Ni~2$p$ core level and valence band, within the same model. The asymmetric line shape as well as the weak intensity feature in the Ni~2$p$ core level spectrum has been ascribed to extrinsic loss processes in the system. The presence of satellite features in the valence band spectrum shows the existence of the lower Hubbard band, deep inside the $pd$ metallic regime, consistent with the predictions of the dynamical mean field theory.
We report the formation and observation of an electron liquid in Sr$_{2-x}$La$_{x}$TiO$_4$, the quasi-two-dimensional counterpart of SrTiO$_3$, through reactive molecular-beam epitaxy and {it in situ} angle-resolved photoemission spectroscopy. The lowest lying states are found to be comprised of Ti 3$d_{xy}$ orbitals, analogous to the LaAlO$_3$/SrTiO$_3$ interface and exhibit unusually broad features characterized by quantized energy levels and a reduced Luttinger volume. Using model calculations, we explain these characteristics through an interplay of disorder and electron-phonon coupling acting co-operatively at similar energy scales, which provides a possible mechanism for explaining the low free carrier concentrations observed at various oxide heterostructures such as the LaAlO$_3$/SrTiO$_3$ interface.
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