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Register a new userDimensional crossover of the electronic structure in LaNiO3 ultrathin films: Orbital reconstruction, Fermi surface nesting, and the origin of the metal-insulator transition
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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.
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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.
SrRuO$_3$ (SRO) films are known to exhibit insulating behavior as their thickness approaches four unit cells. We employ electron energy$-$loss (EEL) spectroscopy to probe the spatially resolved electronic structures of both insulating and conducting SRO to correlate them with the metal$-$insulator transition (MIT). Importantly, the central layer of the ultrathin insulating film exhibits distinct features from the metallic SRO. Moreover, EEL near edge spectra adjacent to the SrTiO$_3$ (STO) substrate or to the capping layer are remarkably similar to those of STO. The site$-$projected density of states based on density functional theory (DFT) partially reflects the characteristics of the spectra of these layers. These results may provide important information on the possible influence of STO on the electronic states of ultrathin SRO.
We present angle-resolved photoemission spectroscopy of Eu(1-x)Gd(x)O through the ferromagnetic metal-insulator transition. In the ferromagnetic phase, we observe Fermi surface pockets at the Brillouin zone boundary, consistent with density functional theory, which predicts a half metal. Upon warming into the paramagnetic state, our results reveal a strong momentum-dependent evolution of the electronic structure, where the metallic states at the zone boundary are replaced by pseudogapped states at the Brillouin zone center due to the absence of magnetic long-range order of the Eu 4f moments.
By means of high-resolution angle resolved photoelectron spectroscopy (ARPES) we have studied the fermiology of 2H transition metal dichalcogenide polytypes TaSe2, NbSe2, and Cu0.2NbS2. The tight-binding model of the electronic structure, extracted from ARPES spectra for all three compounds, was used to calculate the Lindhard function (bare spin susceptibility), which reflects the propensity to charge density wave (CDW) instabilities observed in TaSe2 and NbSe2. We show that though the Fermi surfaces of all three compounds possess an incommensurate nesting vector in the close vicinity of the CDW wave vector, the nesting and ordering wave vectors do not exactly coincide, and there is no direct relationship between the magnitude of the susceptibility at the nesting vector and the CDW transition temperature. The nesting vector persists across the incommensurate CDW transition in TaSe2 as a function of temperature despite the observable variations of the Fermi surface geometry in this temperature range. In Cu0.2NbS2 the nesting vector is present despite different doping level, which lets us expect a possible enhancement of the CDW instability with Cu-intercalation in the CuxNbS2 family of materials.
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.
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