6 research outputs found
Nature of the metallic and in-gap states in Ni-doped SrTiO
Epitaxial thin films of SrTiO(100) doped with 6% and 12% Ni are studied
with resonant angle-resolved photoelectron spectroscopy (ARPES) at the Ti and
Ni L2,3-edges. We find that the Ni doping shifts the valence band (VB) of
pristine SrTiO towards the Fermi level (p-doping) and reduces its band gap.
This is accompanied by an upward energy shift of the Ti t2g-derived mobile
electron system (MES). Thereby, the in-plane dxy-derived bands reduce the
embedded electron density, as evidenced by progressive reduction of their Fermi
momentum with the Ni concentration, and the out-of-plane dxz/yz-derived bands
depopulate, making the MES purely two-dimensional. Furthermore, the Ti and Ni
L2,3-edge resonant photoemission is used to identify the Ni 3d impurity state
in the vicinity of the valence-band maximum, and decipher the full spectrum of
the VO-induced in-gap states originating from the Ni atoms, Ti atoms, and from
their hybridized orbitals. Our experimental information about the dependence of
the valence bands, MES and in-gap states in Ni-doped SrTiO may help
development of this material towards its device applications associated with
the reduced optical band gap
Nature of the metallic and in-gap states in Ni-doped SrTiO
International audienceEpitaxial thin films of SrTiO (100) doped with 6% and 12% Ni are studied with resonant angle-resolved photoelectron spectroscopy at the Ti and Ni L-edges. We find that the Ni doping shifts the valence band of n-doped pristine SrTiO toward the Fermi level (in the direction of p-doping) and reducing the bandgap. In the Ti t-derived mobile electron system (MES), the Ni doping depopulates the out-of-plane d-derived bands, transforming the MES to two-dimensional and progressively reduces the electron density embedded in the in-plane dxy-derived bands as reflected in their Fermi momentum. Furthermore, the Ti and Ni L-edge resonant photoemission is used to identify the Ni 3d impurity state in the vicinity of the valence-band maximum and decipher the full spectrum of the in-gap states originating from the Ni atoms, Ti atoms, and from their hybridized orbitals. Our experimental information about the dependence of the valence bands, MES, and in-gap states in Ni-doped SrTiO may help the development of this material toward its device applications associated with the reduced optical bandgap
Toward Functionalized Ultrathin Oxide Films: The Impact of Surface Apical Oxygen
Thin films of transition metal oxides open up a gateway to nanoscale electronic devices beyond silicon characterized by novel electronic functionalities. While such films are commonly prepared in an oxygen atmosphere, they are typically considered to be ideally terminated with the stoichiometric composition. Using the prototypical correlated metal SrVO as an example, it is demonstrated that this idealized description overlooks an essential ingredient: oxygen adsorbing at the surface apical sites. The oxygen adatoms, which are present even if the films are kept in an ultrahigh vacuum environment and not explicitly exposed to air, are shown to severely affect the intrinsic electronic structure of a transition metal oxide film. Their presence leads to the formation of an electronically dead surface layer but also alters the band filling and the electron correlations in the thin films. These findings highlight that it is important to take into account surface apical oxygen or—mutatis mutandis—the specific oxygen configuration imposed by a capping layer to predict the behavior of ultrathin films of transition metal oxides near the single unit-cell limit
Photoemission study of pristine and Ni-doped SrTiO 3 thin films
International audienceWe combined photoelectron spectroscopy with first-principles calculations to investigate electronic properties of SrTiO3 doped with Ni impurities. High-quality epitaxial pristine SrTiO3 and SrTiO3:Nix films with x =0.06 and 0.12 were prepared by pulsed laser deposition. Electronic band structure calculations for the ground state, as well as one-step model photoemission calculations, which were obtained by means of the Korringa-Kohn-Rostoker Green's function method, predict the formation of localized 3 d -impurity bands in the band gap of SrTiO3 close to the valence band maxima. The measured valence bands at the resonance Ni 2 p excitation and band dispersion confirm these findings
Hard x-ray angle-resolved photoemission from a buried high-mobility electron system
Novel two-dimensional electron systems at the interfaces and surfaces of transition-metal oxides recently have attracted much attention as they display tunable, intriguing properties that can be exploited in future electronic devices. Here we show that a high-mobility quasi-two-dimensional electron system with strong spin-orbit coupling can be induced at the surface of a KTaO (001) crystal by pulsed laser deposition of a disordered LaAlO film. The momentum-resolved electronic structure of the buried electron system is mapped out by hard x-ray angle-resolved photoelectron spectroscopy. From a comparison to calculations, it is found that the band structure deviates from that of electron-doped bulk KTaO due to the confinement to the interface. Fermi surface mapping shows a three-dimensional, periodic intensity pattern consistent with electron pockets of quantum well states centered around the Γ points and the expectations from a Fourier analysis-based description of photoemission on confined electron systems. From the k broadening of the Fermi surface and core-level depth profiling, we estimate the extension of the electron system to be at least 1 nm but not much larger than 2 nm, respectively
Hard x-ray angle-resolved photoemission from a buried high-mobility electron system
Novel two-dimensional electron systems at the interfaces and surfaces of transition-metal oxides recently have attracted much attention as they display tunable, intriguing properties that can be exploited in future electronic devices. Here we show that a high-mobility quasi-two-dimensional electron system with strong spin-orbit coupling can be induced at the surface of a KTaO (001) crystal by pulsed laser deposition of a disordered LaAlO film. The momentum-resolved electronic structure of the buried electron system is mapped out by hard x-ray angle-resolved photoelectron spectroscopy. From a comparison to calculations, it is found that the band structure deviates from that of electron-doped bulk KTaO due to the confinement to the interface. Fermi surface mapping shows a three-dimensional, periodic intensity pattern consistent with electron pockets of quantum well states centered around the Γ points and the expectations from a Fourier analysis-based description of photoemission on confined electron systems. From the k broadening of the Fermi surface and core-level depth profiling, we estimate the extension of the electron system to be at least 1 nm but not much larger than 2 nm, respectively