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Metal-insulator transition in ultrathin LaNiO3 films

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 Added by Raoul Scherwitzl
 Publication date 2011
  fields Physics
and research's language is English




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Transport in ultrathin films of LaNiO3 evolves from a metallic to a strongly localized character as the films thickness is reduced and the sheet resistance reaches a value close to h/e2, the quantum of resistance in two dimensions. In the intermediate regime, quantum corrections to the Drude low- temperature conductivity are observed; they are accurately described by weak localization theory. Remarkably, the negative magnetoresistance in this regime is isotropic, which points to magnetic scattering associated with the proximity of the system to either a spin glass state or the charge ordered antiferromagnetic state observed in other rare earth nickelates.



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The nature of the metal insulator transition in thin films and superlattices of LaNiO3 with only few unit cells in thickness remains elusive despite tremendous effort. Quantum confinement and epitaxial strain have been evoked as the mechanisms, although other factors such as growth-induced disorder, cation non-stoichiometry, oxygen vacancies, and substrate-film interface quality may also affect the observable properties in the ultrathin films. Here we report results obtained for near-ideal LaNiO3 films with different thicknesses and terminations grown by atomic layer-by-layer laser molecular beam epitaxy on LaAlO3 substrates. We find that the room-temperature metallic behavior persists until the film thickness is reduced to an unprecedentedly small 1.5 unit cells (NiO2 termination). Electronic structure measurements using x-ray absorption spectroscopy and first-principles calculation suggest that oxygen vacancies existing in the films also contribute to the metal insulator transition.
The spin relaxation induced by the Elliott-Yafet mechanism and the extrinsic spin Hall conductivity due to the skew-scattering are investigated in 5d transition-metal ultrathin films with self-adatom impurities as scatterers. The values of the Elliott-Yafet parameter and of the spin-flip relaxation rate reveal a correlation with each other that is in agreement with the Elliott approximation. At 10-layer thickness, the spin-flip relaxation time in 5d transition-metal films is quantitatively reported about few hundred nanoseconds at atomic percent which is one and two orders of magnitude shorter than that in Au and Cu thin films, respectively. The anisotropy effect of the Elliott-Yafet parameter and of the spin-flip relaxation rate with respect to the direction of the spin-quantization axis in relation to the crystallographic axes is also analyzed. We find that the anisotropy of the spin-flip relaxation rate is enhanced due to the Rashba surface states on the Fermi surface, reaching values as high as 97% in 10-layer Hf(0001) film or 71% in 10-layer W(110) film. Finally, the spin Hall conductivity as well as the spin Hall angle due to the skew-scattering off self-adatom impurities are calculated using the Boltzmann approach. Our calculations employ a relativistic version of the first-principles full-potential Korringa-Kohn-Rostoker Green function method.
Metallic oxide SrVO3 represents a prototype system for the study of the mechanism behind thickness-induced metal-to-insulator transition (MIT) or crossover in thin films due to its simple cubic symmetry with one electron in the 3d state in the bulk. Here we report a deviation of chemical composition and distortion of lattice structure existing in the initial 3 unit cells of SrVO3 films grown on SrTiO3 (001) from its bulk form, which shows a direct correlation to the thickness-dependent MIT. In-situ photoemission and scanning tunneling spectroscopy indicate a MIT at the critical thickness of ~3 unit cell (u.c.), which coincides with the formation of a (root2Xroot2)R45 surface reconstruction. However, atomically resolved scanning transmission electron microscopy and electron energy loss spectroscopy show depletion of Sr, change of V valence, thus implying the existence of a significant amount of oxygen vacancies in the 3 u.c. of SrVO3 near the interface. Transport and magneto-transport measurements further reveal that disorder, rather than electron correlations, is likely to be the main cause for the MIT in the SrVO3 ultrathin films.
Dimensionality control in the LaNiO3 (LNO) heterostructure has attracted attention due to its two-dimensional (2D) electronic structure was predicted to have an orbital ordered insulating ground state, analogous to that of the parent compound of high-Tc cuprate superconductors [P. Hansmann et al., Phys. Rev. Lett. 103, 016401 (2009)]. Here, we directly measured the electronic structure of LNO ultrathin films using in situ angle-resolved photoemission spectroscopy (ARPES). We recognized the dimensional crossover of the electronic structure around 3-unit cells (UC)-thick LNO film and observed the orbital reconstruction. However, complete orbital ordering was not achieved. Instead, we observed that the Fermi surface nesting effect became strong in the 2D LNO ultrathin film. These results indicated that the orbital reconstruction should be described by taking into account the strong nesting effect to search for the novel phenomena, such as superconductivity in 2D LNO heterostructure. In addition, the APRES spectra showed that the Fermi surface existed down to a 1-UC-thick film, which showed insulating behavior in transport measurements. We suggested that the metal-insulator transition in the transport properties may originate from Anderson localization.
Fundamental understanding of interfacial magnetic properties in ferromagnetic heterostructures is essential to utilize ferromagnetic materials for spintronic device applications. In this paper, we investigate the interfacial magnetic and electronic structures of epitaxial single-crystalline LaAlO$_3$ (LAO)/La$_{0.6}$Sr$_{0.4}$MnO$_3$ (LSMO)/Nb:SrTiO$_3$ (Nb:STO) heterostructures with varying LSMO-layer thickness, in which the magnetic anisotropy strongly changes depending on the LSMO thickness due to the delicate balance between the strains originating from both the Nb:STO and LAO layers, using x-ray magnetic circular dichroism (XMCD) and photoemission spectroscopy (PES). We successfully detect the clear change of the magnetic behavior of the Mn ions concomitant with the thickness-dependent metal-insulator transition (MIT). Our results suggest that double-exchange interaction induces the ferromagnetism in the metallic LSMO film under tensile strain caused by the SrTiO$_3$ substrate, while superexchange interaction determines the magnetic behavior in the insulating LSMO film under compressive strain originating from the top LAO layer. Based on those findings, the formation of a magnetic dead layer near the LAO/LSMO interface is attributed to competition between the superexchange interaction via Mn 3$d_{3z^2-r^2}$ orbitals under compressive strain and the double-exchange interaction via the 3$d_{x^2-y^2}$ orbitals.
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