The band structure and Fermi surface of La0.6_{0.6}Sr0.4_{0.4}MnO3_{3} thin films studied by in-situ angle-resolved photoemission spectroscopy

We have performed an in situ angle-resolved photoemission spectroscopy (ARPES) on single-crystal surfaces of La$_{0.6}$Sr$_{0.4}$MnO$_{3}$ (LSMO) thin films grown on SrTiO$_{3}$ (001) substrates by laser molecular beam epitaxy, and investigated the electronic structure near the Fermi level ($E_{F}$). The experimental results were compared with the band-structure calculation based on LDA + $U$. The band structure of LSMO thin films consists of several highly dispersive O 2$p$ derived bands in the binding energy range of 2.0 - 6.0 eV and Mn 3$d$ derived bands near $E_{F}$. ARPES spectra around the $Gamma$ point show a dispersive band near $E_{F}$ indicative of an electron pocket centered at the $Gamma$ point, although it was not so clearly resolved as an electronlike pocket due to the suppression of spectral weight in the vicinity of $E_{F}$. Compared with the band-structure calculation, the observed conduction band is assigned to the Mn 3$de_{g}$ majority-spin band responsible for the half-metallic nature of LSMO. We have found that the estimated size of the Fermi surface is consistent with the prediction of the band-structure calculation, while the band width becomes significantly narrower than the calculation. Also, the intensity near $E_{F}$ is strongly reduced. The origin of these discrepancies between the experiment and the calculation is discussed.Comment: 7 pages, 5 figure

In situ photoemission study on atomically-controlled La1−x_{1-x}Srx_xMnO3_3 thin films: Composition dependence of the electronic structure

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.Comment: 8 pages, 8 figure

In-situ photoemission study of Pr_{1-x}Ca_xMnO_3 epitaxial thin films with suppressed charge fluctuations

We have performed an {\it in-situ} photoemission study of Pr_{1-x}Ca_xMnO_3 (PCMO) thin films grown on LaAlO_3 (001) substrates and observed the effect of epitaxial strain on the electronic structure. We found that the chemical potential shifted monotonically with doping, unlike bulk PCMO, implying the disappearance of incommensurate charge fluctuations of bulk PCMO. In the valence-band spectra, we found a doping-induced energy shift toward the Fermi level (E_F) but there was no spectral weight transfer, which was observed in bulk PCMO. The gap at E_F was clearly seen in the experimental band dispersions determined by angle-resolved photoemission spectroscopy and could not be explained by the metallic band structure of the C-type antiferromagnetic state, probably due to localization of electrons along the ferromagnetic chain direction or due to another type of spin-orbital ordering.Comment: 5 pages, 4 figure

Angle-resolved photoemission spectroscopy of perovskite-type transition-metal oxides and their analyses using tight-binding band structure

Nowadays it has become feasible to perform angle-resolved photoemission spectroscopy (ARPES) measurements of transition-metal oxides with three-dimensional perovskite structures owing to the availability of high-quality single crystals of bulk and epitaxial thin films. In this article, we review recent experimental results and interpretation of ARPES data using empirical tight-binding band-structure calculations. Results are presented for SrVO$_3$ (SVO) bulk single crystals, and La$_{1-x}$Sr$_x$FeO$_3$ (LSFO) and La$_{1-x}$Sr$_x$MnO$_3$ (LSMO) thin films. In the case of SVO, from comparison of the experimental results with calculated surface electronic structure, we concluded that the obtained band dispersions reflect the bulk electronic structure. The experimental band structures of LSFO and LSMO were analyzed assuming the G-type antiferromagnetic state and the ferromagnetic state, respectively. We also demonstrated that the intrinsic uncertainty of the electron momentum perpendicular to the crystal surface is important for the interpretation of the ARPES results of three-dimensional materials.Comment: 25 pages, 12 figure

Manifestation of Correlation Effects in the photoemission spectra of Ca1−x_{1-x}Srx_xRuO3_3

We have measured soft x-ray photoemission and O 1{\it s} x-ray absorption spectra of Ca$_{1-x}$Sr$_x$RuO$_3$ thin films prepared {\it in situ}. The coherent and incoherent parts have been identified in the bulk component of the photoemission spectra, and spectral weight transfer from the coherent to the incoherent part has been observed with decreasing $x$, namely, with increasing orthorhombic distortion. We propose that, while the Ru 4d one-electron bandwidth does not change with $x$, the distortion and hence the splitting of the $t_{2\text{g}}$ band effectively increases electron correlation strength. Although strong mass enhancement is found in the electronic specific heat data, the coherent part remains wide, suggesting enhanced band narrowing only in the vicinity of {\it E$_{F}$}

Gradual Disappearance of the Fermi Surface near the Metal-Insulator Transition in La1−x_{1-x}Srx_{x}MnO3_{3}

We report the first observation of changes in the electronic structure of La$_{1-x}$Sr$_{x}$MnO$_{3}$ (LSMO) across the filling-control metal-insulator (MI) transition by means of in situ angle-resolved photoemission spectroscopy (ARPES) of epitaxial thin films. The Fermi surface gradually disappears near the MI transition by transferring the spectral weight from the coherent band near the Fermi level ($E_{F}$) to the lower Hubbard band, whereas a pseudogap behavior also exists in the ARPES spectra in the close vicinity of $E_{F}$ for the metallic LSMO. These results indicate that the spectral weight transfer derived from strong electron-electron interaction dominates the gap formation in LSMO associated with the filling-control MI transition.Comment: 11 pages, 4 figure

Madelung potentials and covalency effect in strained La1−x_{1-x}Srx_xMnO3_3 thin films studied by core-level photoemission spectroscopy

We have investigated the shifts of the core-level photoemission spectra of La$_{0.6}$Sr$_{0.4}$MnO$_3$ thin films grown on three kinds of substrates, SrTiO$_3$, (LaAlO$_3$)$_{0.3}$-(SrAl$_{0.5}$Ta$_{0.5}$O$_3$)$_{0.7}$, and LaAlO$_3$. The experimental shifts of the La 4d and Sr 3d core levels are almost the same as the calculation, which we attribute to the absence of covalency effects on the Madelung potentials at these atomic sites due to the nearly ionic character of these atoms. On the other hand, the experimental shifts of the O $1s$ and Mn $2p$ core levels are negligibly small, in disagreement with the calculation. We consider that this is due to the strong covalent character of the Mn-O bonds.Comment: 4 pages, 5 figure

Photoemission study of TiO2/VO2 interfaces

We have measured photoemission spectra of two kinds of TiO$_2$-capped VO$_2$ thin films, namely, that with rutile-type TiO$_2$ (r-TiO$_2$/VO$_2$) and that with amorphous TiO$_2$ (a-TiO$_2$/VO$_2$) capping layers. Below the Metal-insulator transition temperature of the VO$_2$ thin films, $\sim 300$ K, metallic states were not observed for the interfaces with TiO$_2$, in contrast with the interfaces between the band insulator SrTiO$_3$ and the Mott insulator LaTiO$_3$ in spite of the fact that both TiO$_2$ and SrTiO$_3$ are band insulators with $d^0$ electronic configurations and both VO$_2$ and LaTiO$_3$ are Mott insulators with $d^1$ electronic configurations. We discuss possible origins of this difference and suggest the importance of the polarity discontinuity of the interfaces. Stronger incoherent part was observed in r-TiO$_2$/VO$_2$ than in a-TiO$_2$/VO$_2$, suggesting Ti-V atomic diffusion due to the higher deposition temperature for r-TiO$_2$/VO$_2$.Comment: 5 pages, 6 figure

Effect of strong localization of doped holes in angle-resolved photoemission spectra of La1−x_{1-x}Srx_xFeO3_3

We have performed an angle-resolved photoemission spectroscopy study of La$_{0.6}$Sr$_{0.4}$FeO$_3$ using {\it in situ} prepared thin films and determined its band structure. The experimental band dispersions could be well explained by an empirical band structure assuming the G-type antiferromagnetic state. However, the Fe 3d bands were found to be shifted downward relative to the Fermi level ($E_F$) by $\sim 1$ eV compared with the calculation and to form a (pseudo)gap of $\sim 1$ eV at $E_F$. We attribute this observation to a strong localization effect of doped holes due to polaron formation.Comment: 5 pages, 5 figure

Direct observation of double valence-band extrema and anisotropic effective masses of the thermoelectric material SnSe

Synchrotron-based angle-resolved photoemission spectroscopy is used to determine the electronic structure of layered SnSe, which was recently turned out to be a potential thermoelectric material. We observe that the top of the valence band consists of two nearly independent hole bands, whose tops differ by ~20 meV in energy, indicating the necessity of a multivalley model to describe the thermoelectric properties. The estimated effective masses are anisotropic, with in-plane values of 0.16-0.39 m$_0$ and an out-of-plane value of 0.71 m$_0$, where m$_0$ is the rest electron mass. Information of the electronic structure is essential to further enhance the thermoelectric performance of hole-doped SnSe.Comment: 14 pages including 2 figures + 2 pages of supplementary dat