Searcharxiv⌕ Search

arXiv subjects

H. Wadati

Publications and source records attributed to H. Wadati.

At least 55 records · Page 3Linked to original sources

Madelung potentials and covalency effect in strained La$_{1-x}$Sr$_x$MnO$_3$ 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.

cond-mat.str-el↗

Systematic tight-binding analysis of ARPES spectra of transition-metal oxides

We have performed systematic tight-binding (TB) analyses of the angle-resolved photoemission spectroscopy (ARPES) spectra of transition-metal (TM) oxides A$M$O$_3$ ($M=$ Ti, V, Mn, and Fe) with the perovskite-type structure and compared the obtained parameters with those obtained from configuration-interaction (CI) cluster-model analyses of photoemission spectra. The values of $ε_d-ε_p$ from ARPES are found to be similar to the charge-transfer energy $Δ$ from O $2p$ orbitals to empty TM 3d orbitals and much larger than $Δ-U/2$ ($U$: on-site Coulomb energy) expected for Mott-Hubbard-type compounds including SrVO$_3$. $ε_d-ε_p$ values from {\it ab initio} band-structure calculations show similar behaviors to those from ARPES. The values of the $p-d$ transfer integrals to describe the global electronic structure are found to be similar in all the estimates, whereas additional narrowing beyond the TB description occurs in the ARPES spectra of the $d$ band.

cond-mat.str-el↗

Electronic structure of the SrTiO$_3$/LaAlO$_3$ interface revealed by resonant soft x-ray scattering

We investigated the electronic structure of the SrTiO$_3$/LaAlO$_3$ superlattice (SL) by resonant soft x-ray scattering. The (003) peak, which is forbidden for our "ideal" SL structure, was observed at all photon energies, indicating reconstruction at the interface. From the peak position analyses taking into account the effects of refraction, we obtained evidence for electronic reconstruction of Ti 3d and O $2p$ states at the interface. From reflectivity analyses, we concluded that the AlO$_2$/LaO/TiO$_2$/SrO and the TiO$_2$/SrO/AlO$_2$/LaO interfaces are quite different, leading to highly asymmetric properties.

cond-mat.str-el↗

Remote hole-doping of Mott insulators on the nanometer scale

At interfaces between polar and nonpolar perovskite oxides, an unusual electron-doping has been previously observed, due to electronic reconstructions. We report on remote hole-doping at an interface composed of only polar layers, revealed by high-resolution hard x-ray core-level photoemission spectroscopy. In LaAlO3/LaVO3/LaAlO3 trilayers, the vanadium valence systematically evolves from the bulk value of V3+ to higher oxidation states with decreasing LaAlO3 cap layer thickness. These results provide a synthetic approach to hole-doping transition metal oxide heterointerfaces without invoking a polar discontinuity.

cond-mat.str-el↗

Bulk-like d band of SrVO3 under a self-protective cap layer

We have performed a detailed angel-resolved photoemission spectroscopy study of in-situ prepared SrVO3 thin films. Naturally capped by a ``transparent'' protective layer, contributions from surface states centered at ~ -1.5 eV are dramatically reduced, enabling us to study the bulk V 3d states. We have observed a clear band dispersion not only in the coherent quasiparticle part but also in the incoherent part, which are reproduced by dynamical mean-field theory calculations and the spectral weight of the incoherent part is stronger within the Fermi surface.

cond-mat.str-el↗

Charge order in La_{1.8-x}Eu_{0.2}Sr_xCuO_4 studied by resonant soft X-ray diffraction

Resonant soft X-ray scattering with photon energies near the O K and the Cu L3 edges was used to study charge ordering in the system La_{1.8-x}Eu_{0.2}Sr_xCuO_4 as a function of temperature for x = 0.125 and 0.15. From the superstructure diffraction intensities a charge ordering with a doping dependent wave vector is derived which is in this system well below the transition temperature of the low-temperature tetragonal phase but well above the onset of spin ordering. This indicates that charge ordering is the primary driving force for the formation of stripe-like phases in two-dimensional doped cuprates. Analysis of the lineshape of the scattered intensity as a function of photon energy yields evidence for a high hole concentration in the stripes.

cond-mat.supr-con↗

Effects of electron-phonon coupling in angle-resolved photoemission spectra of SrTiO3

We have studied the O 2p valence-band structure of Nb-doped SrTiO3, in which a dilute concentration of electrons are doped into the d0 band insulator, by angle-resolved photoemission spectroscopy (ARPES) measurements. We found that ARPES spectra at the valence band maxima at the M [k = (pi/a, pi/a, 0)]and R [k = (pi/a, pi/a, pi/a)] points start from ~ 3.3 eV below the Fermi level (EF), consistent with the indirect band gap of 3.3 eV and the EF position at the bottom of the conduction band. The peak position of the ARPES spectra were, however, shifted toward higher binding energies by ~ 500 meV from the 3.3 eV threshold. Because the bands at M and R have pure O 2p character, we attribute this ~ 500 meV shift to strong coupling of the oxygen p hole with optical phonons in analogy with the peak shifts observed for d-electron photoemission spectra in various transition-metal oxides.

cond-mat.mtrl-sci↗

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.

cond-mat.str-el↗

Phase Change Observed in Ultrathin Ba0.5Sr0.5TiO3 Films by in-situ Resonant Photoemission Spectroscopy

Epitaxial Ba0.5Sr0.5TiO3 thin films were prepared on Nb-doped SrTiO3 (100)substrates by the pulsed laser deposition technique, and were studied by measuring the Ti 2p - 3d resonant photoemission spectra in the valence-band region as a function of film thickness, both at room temperature and low temperature. Our results demonstrated an abrupt variation in the spectral structures between 2.8 nm (~7 monolayers) and 2.0 nm (~5 monolayers) Ba0.5Sr0.5TiO3 films, suggesting that there exists a critical thickness for phase change in the range of 2.0 nm to 2.8 nm. This may be ascribed mainly to the intrinsic size effects.

cond-mat.mtrl-sci↗

Gradual Disappearance of the Fermi Surface near the Metal-Insulator Transition in La$_{1-x}$Sr$_{x}$MnO$_{3}$

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.

cond-mat.str-el↗

Hard x-ray photoemission study of LaAlO3/LaVO3 multilayers

We have studied the electronic structure of multilayers composed of a band insulator LaAlO$_3$ (LAO) and a Mott insulator LaVO$_3$ (LVO) by means of hard x-ray photoemission spectroscopy, which has a probing depth as large as $\sim 60 Å$. The Mott-Hubbard gap of LVO remained open at the interface, indicating that the interface is insulating unlike the LaTiO$_3$/SrTiO$_3$ multilayers. We found that the valence of V in LVO were partially converted from V$^{3+}$ to V$^{4+}$ only at the interface on the top side of the LVO layer and that the amount of V$^{4+}$ increased with LVO layer thickness. We suggest that the electronic reconstruction to eliminate the polarity catastrophe inherent in the polar heterostructure is the origin of the highly asymmetric valence change at the LVO/LAO interfaces.

cond-mat.str-el↗

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$_2$.

cond-mat.str-el↗

Electronic structure of the Mott insulator LaVO3 in a quantum well geometry

We used x-ray photoemission spectroscopy to investigate the electronic structure of the Mott insulator LaVO3 embedded in LaAlO3. By limiting the upper layer of LaAlO3 to 3 unit cells, the underlying LaVO3 could be probed. The V 2p core-level spectra had both V3+ and V4+ components, and above 2 unit cell thick LaVO3, the structures exhibited spectra similar to bulk samples. The atomically flat surfaces enabled study of the emission angle dependence, which indicates the V4+ is localized to the topmost layer. These results demonstrate the potential for probing interface electronic structure in oxide ultrathin films by surface spectroscopy.

cond-mat.mtrl-sci↗

Chemical potential shift and spectral weight transfer in Pr$_{1-x}$Ca$_x$MnO$_3$ revealed by photoemission spectroscopy

We have studied the chemical potential shift and changes in the electronic density of states near the Fermi level ($E_F$) as a function of carrier concentration in Pr$_{1-x}$Ca$_x$MnO$_3$ (PCMO, $0.2 \le x \le 0.65$) through the measurements of photoemission spectra. The results showed that the chemical potential shift was suppressed for $x \agt 0.3$, where the charge exchange (CE)-type antiferromagnetic charge-ordered state appears at low temperatures. We consider this observation to be related to charge self-organization such as stripe formation on a microscopic scale in this composition range. Together with the previous observation of monotonous chemical potential shift in La$_{1-x}$Sr$_x$MnO$_3$, we conclude that the tendency toward the charge self-organization increases with decreasing bandwidth. In the valence band, spectral weight of the Mn 3$d$ $e_g$ electrons in PCMO was transferred from $\sim$ 1 eV below $E_F$ to the region near $E_F$ with hole doping, leading to a finite intensity at $E_F$ even in the paramagnetic insulating phase for $x \agt 0.3$, probably related with the tendency toward charge self-organization. The finite intensity at $E_F$ in spite of the insulating transport behavior is consistent with fluctuations involving ferromagnetic metallic states.

cond-mat.str-el↗

Photoemission from buried interfaces in SrTiO3/LaTiO3 superlattices

We have measured photoemission spectra of SrTiO3/LaTiO3 superlattices with a topmost SrTiO3 layer of variable thickness. Finite coherent spectral weight with a clear Fermi cut-off was observed at chemically abrupt SrTiO3/LaTiO3 interfaces, indicating that an ``electronic reconstruction'' occurs at the interface between the Mott insulator LaTiO3 and the band insulator SrTiO3. For SrTiO3/LaTiO3 interfaces annealed at high temperatures (~ 1000 C), which leads to Sr/La atomic interdiffusion and hence to the formation of La1-xSrxTiO3-like material, the intensity of the incoherent part was found to be dramatically reduced whereas the coherent part with a sharp Fermi cut-off is enhanced due to the spread of charge. These important experimental features are well reproduced by layer dynamical-mean-field-theory calculation.

cond-mat.mtrl-sci↗

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.

cond-mat.str-el↗

Effect of strong localization of doped holes in angle-resolved photoemission spectra of La$_{1-x}$Sr$_x$FeO$_3$

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.

cond-mat.str-el↗

Robust Ti4+ states in SrTiO3 layers of La0.6Sr0.4MnO3/SrTiO3/ La0.6Sr0.4MnO3 junctions

We have investigated the interfacial electronic structure of La0.6Sr0.4MnO3 (LSMO)/ SrTiO3 (STO)/ LSMO heterojunctions utilizing the elemental selectivity of photoemission spectroscopy. The Ti 2p core-level spectra clearly show Ti4+ states and do not exhibit any indication of Ti3+ states in TiO2 layers irrespective of a different kind of adjacent atomic layer with different chemical carrier concentration. This result indicates that the Ti ions in the TiO2 atomic layers preserve their tetravalent states even in the vicinity of the valence-mismatched interface between LSMO and STO, reflecting chemical stability of the Ti4+ states.

cond-mat.str-el↗