arXiv subjects

M. Lippmaa

Publications and source records attributed to M. Lippmaa.

At least 19 recordsLinked to original sources

arXiv2015

A-site driven ferroelectricity in strained ferromagnetic L2NiMnO6 thin films

We report on theoretical and experimental investigation of A-site driven ferroelectricity in ferromagnetic La2NiMnO6 thin films grown on SrTiO3 substrates. Structural analysis and density functional theory calculations show that epitaxial strain stretches the rhombohedral La2NiMnO6 crystal lattice along the [111]cubic direction, triggering a displacement of the A-site La ions in the double perovskite lattice. The lattice distortion and the A-site displacements stabilize a ferroelectric polar state in ferromagnetic La2NiMnO6 crystals. The ferroelectric state only appears in the rhombohedral La2NiMnO6 phase, where MnO6 and NiO6 octahedral tilting is inhibited by the 3-fold crystal symmetry. Electron localization mapping showed that covalent bonding with oxygen and 6s orbital lone pair formation are negligible in this material.

cond-mat.mtrl-sci↗

arXiv2013

Spectroscopic studies on the electronic and magnetic states of Co-doped perovskite manganite Pr0.8Ca0.2Mn1-yCoyO3 thin films

We have investigated the electronic and magnetic properties of Co-doped Pr0.8Ca0.2MnO3 thin films using various spectroscopic techniques. X-ray absorption and hard x-ray photoemission spectroscopy revealed that the substituted Co ions are in the divalent state, resulting in hole doping on the Mn atoms. Studies of element-selective magnetic properties by x-ray magnetic circular dichroism found a large orbital magnetic moment for the Co ions. These spectroscopic studies reveal that the substituted Co ions play several roles of hole doping for Mn, ferromagnetic superexchange coupling between the Co2+ and Mn4+ ions, and orbital magnetism of the Co2+ ions. Competition among these complex interactions produces the unique electronic and magnetic behaviors including enhanced coercivity of the Co-doped Pr0.8Ca0.2MnO3.

cond-mat.str-el↗

arXiv2012

Pyroelectric detection of spontaneous polarization in magnetite thin films

We have investigated the spontaneous polarization in Fe$_3$O$_4$ thin films by using dynamic and static pyroelectric measurements. The magnetic and dielectric behavior of Fe$_3$O$_4$ thin films grown on Nb:SrTiO$_3$(001) substrates was consistent with bulk crystals. The well-known metal-insulator (Verwey) transition was observed at 120 K. The appearance of a pyroelectric response in the Fe$_3$O$_4$ thin films just below the Verwey temperature shows that spontaneous polarization appeared in Fe$_3$O$_4$ at the charge ordering transition temperature. The polar state characteristics are consistent with bond- and site- centered charge ordering of Fe$^{2+}$ and Fe$^{3+}$ ions sharing the octahedral $B$ sites. The pyroelectric response in Fe$_3$O$_4$ thin films was dependent on the dielectric constant. Quasi-static pyroelectric measurement of Pd/Fe$_3$O$_4$/Nb:SrTiO$_3$ junctions showed that magnetite has a very large pyroelectric coefficient of 735 nC/cm$^{2}$K at 60 K.

cond-mat.mtrl-sci↗

arXiv2012

Spin-filter tunnel junction with matched Fermi surfaces

Efficient injection of spin-polarized current into a semiconductor is a basic prerequisite for building semiconductor-based spintronic devices. Here, we use inelastic electron tunneling spectroscopy to show that the efficiency of spin-filter-type spin injectors is limited by spin scattering of the tunneling electrons. By matching the Fermi-surface shapes of the current injection source and target electrode material, spin injection efficiency can be significantly increased in epitaxial ferromagnetic insulator tunnel junctions. Our results demonstrate that not only structural but also Fermi-surface matching is important to suppress scattering processes in spintronic devices.

cond-mat.mtrl-sci↗

arXiv2010

Modulation of the ferromagnetic insulating phase in Pr0.8Ca0.2MnO3 by Co substitution

Ferromagnetic insulator Pr0.8Ca0.2Mn1-yCoyO3 (0 <= y <= 0.7) thin films were epitaxially grown on (LaAlO3)0.3-(SrAl0.5Ta0.5O3)0.7 (100) substrates by pulsed laser deposition. To probe the ferromagnetic insulator state of hole-doped manganites, the Co content dependences of the structural, magnetic, and transport properties were studied. Variation of lattice constant by the substitution of Co ions is well reproduced considering that divalent and trivalent Co ions substitute for Mn ions at the perovskite B-sites. For 0 <= y <= 0.3, the Curie temperature, saturation magnetization, and magnetoresistance increase with increasing Co content, retaining the insulating properties. Detailed analyses of transport and magnetic properties indicate the contribution of both double exchange and superexchange interactions to the appearance of the ferromagnetic insulating phase.

cond-mat.mtrl-sci↗

arXiv2008

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↗

arXiv2007

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↗

arXiv2007

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↗

arXiv2006

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↗

arXiv2006

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↗

arXiv2005

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↗

arXiv2005

Epitaxial growth and transport properties of Nb-doped SrTiO$_{3}$ thin films

Nb-doped SrTiO$_{3}$ epitaxial thin films have been prepared on (001) SrTiO$_{3}$ substrates using pulsed laser deposition. A high substrate temperature ($>1000^{\circ}{C}$) was found to be necessary to achieve 2-dimensional growth. Atomic force microscopy reveals atomically flat surfaces with 3.9 \AA $ $ steps. The films show a metallic behavior, residual resistivity ratios between 10 and 100, and low residual resistivity of the order of 10$^{-4}$$\Omega$cm. At 0.3 K, a sharp superconducting transition, reaching zero resistance, is observed.

cond-mat.supr-con↗

arXiv2005

High Throughput Oxide Lattice Engineering by Parallel Laser Molecular Beam Epitaxy and Concurrent X-ray Diffraction

A novel laser molecular beam epitaxy (LMBE) system for the fabrication of atomically controlled oxides superlattices and an x-ray diffractometer that measures spatially-resolved x-ray diffraction spectra have been developed based on the concept of combinatorial methodology. The LMBE chamber has two moving masks, an automated target stage, a substrate heating laser, and an in-situ scanning reflection high-energy electron diffraction system. The x-ray diffractometer with a curved monochromator and two-dimensional detector is used for rapid concurrent x-ray diffraction intensity mapping with the two axes of the detector corresponding to the diffraction angle and a position in the sample.

cond-mat.mtrl-sci↗

arXiv2005

The band structure and Fermi surface of La$_{0.6}$Sr$_{0.4}$MnO$_{3}$ 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.

cond-mat.str-el↗

arXiv2004

Manifestation of Correlation Effects in the photoemission spectra of Ca$_{1-x}$Sr$_x$RuO$_3$

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$_{F}$}.

cond-mat.str-el↗

arXiv2004

Nature of Well-Screened State in Hard X-ray Mn 2$p$ Core-Level Photoemission of La$_{1-x}$Sr$_x$MnO$_3$ Films

Using hard x-ray (HX ; $hν$ = 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 ; $hν$ $\sim$ 1000 eV) -PES shows a clear additional well-screened feature only in HX-PES. Take-off-angle dependent data indicate its bulk ($\ge$ 20 Å) 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.

cond-mat.str-el↗

arXiv2004

Temperature-dependent soft x-ray photoemission and absorption studies of charge disproportionation in La$_{1-x}$Sr$_x$FeO$_3$

We have measured the temperature dependence of the photoemission and x-ray absorption spectra of La$_{1-x}$Sr$_x$FeO$_3$ (LSFO) epitaxial thin films with $x=0.67$, where charge disproportionation ($3{Fe}^{3.67+}\to 2{Fe}^{3+}+ {Fe}^{5+}$) resulting in long-range spin and charge ordering is known to occur below $T_{CD}=190$ K. With decreasing temperature we observed gradual changes of the spectra with spectral weight transfer over a wide energy range of $\sim 5$ eV. Above $T_{CD}$ the intensity at the Fermi level ($E_F$) was relatively high compared to that below $T_{CD}$ but still much lower than that in conventional metals. We also found a similar temperature dependence for $x=0.4$, and to a lesser extent for $x=0.2$. These observations suggest that a local charge disproportionation occurs not only in the $x=0.67$ sample below $T_{CD}$ but also over a wider temperature and composition range in LSFO. This implies that the tendency toward charge disproportionation may be the origin of the unusually wide insulating region of the LSFO phase diagram.

cond-mat.str-el↗

arXiv2004

In situ photoemission study on atomically-controlled La$_{1-x}$Sr$_x$MnO$_3$ 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.

cond-mat.str-el↗