Dimensional crossover of the electronic structure in LaNiO3 ultrathin films: Orbital reconstruction, Fermi surface nesting, and the origin of the metal-insulator transition (original) (raw)

Dimensionality control in the LaNiO 3 (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-T c 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.

Sign up to get access to over 50M papers

Sign up for access to the world's latest research

Insulating state of ultrathin epitaxial LaNiO_ {3} thin films detected by hard x-ray photoemission

2011

In order to understand the influence of strain and film thickness on the electronic structure of thin films of strongly correlated oxides, we have applied hard x-ray photoemission (HXPS) at 6 keV, soft x-ray photoemission (XPS) at 1.5 keV, and transmission electron microscopy to epitaxial LaNiO 3 films deposited on two substrates: LaAlO 3 (compressive strain) and (LaAlO 3) 0.3 (Sr 2 AlTaO 6) 0.7 (tensile strain). Using inelastic attenuation lengths in LaNiO 3 determined from the HXPS data, we have decomposed valence-band spectra into layer-specific contributions. This decomposition is validated by comparing with the results of first-principles calculations using a hybrid functional. The resultant thin-film LaNiO 3 densities of states exhibit significant differences in spectral weights for the thinnest LaNiO 3 films. A gap opening consistent with a metal-to-insulator transition is observed for the thinnest 2.7 nm LaNiO 3 film on an (LaAlO 3) 0.3 (Sr 2 AlTaO 6) 0.7 substrate, with a similar gap opening also being observed in complementary soft x-ray photoemission at 1.5 keV for a thinner 1.4 nm film on an LaAlO 3 substrate. A metal-to-insulator transition in very thin nm-scale films of LaNiO 3 is thus suggested as a general phenomenon.

Valence band study of LaNiO 3 - d thin films

Keywords: Rare-earth alloys and compounds Resonance photoemission Valence band electronic structure Oxide materials a b s t r a c t The resonant photoemission spectroscopy was used to study the surface electronic structure under La 4d-4f and Ni 3p-3d photo-excitation of thin LaNiO 3 À d films after annealing in ultrahigh vacuum above dehydration temperature. The giant resonance in La 5p and La 5s peaks intensity observed at excitation energy corresponding to a La 4d-4f threshold is accompanied by resonance of the N 4,5 O 2,3 O 2,3 and N 4,5 O 2,3 V Auger peaks. The enhancement in the intensity of valence band maxima (at about 6 eV) may be explained by the small mixing of the La 5d ionic character to the O 2p valence band. The week resonant features observed in the valence band spectra under Ni 3p-3d threshold indicate the loss of nickel species at the LaNiO 3 À d film surface after heat treatment.

Quantum confinement of Mott electrons in ultrathin LaNiO_{3}/LaAlO_{3} superlattices

Physical Review B, 2011

We investigate the electronic reconstruction in (LaNiO3)n/(LaAlO3)3 (n =3, 5 and 10) superlattices due to the quantum confinement (QC) by d.c. transport and resonant soft x-ray absorption spectroscopy. In proximity to the QC limit, a Mott-type transition from an itinerant electron behavior to a localized state is observed. The system exhibits tendency towards charge-order during the transition. ab initio cluster calculations are in good agreement with the absorption spectra, indicating that the apical ligand hole density is highly suppressed resulting in a strong modification of the electronic structure. At the dimensional crossover cellular dynamicalmean-field calculations support the emergence of a Mott insulator ground state in the heterostructured ultra-thin slab of LaNiO3.

Confinement-induced metal-to-insulator transition in strained LaNiO_{3}/LaAlO_{3} superlattices

Physical Review B, 2011

Using density functional theory calculations including a Hubbard U term we explore the effect of strain and confinement on the electronic ground state of superlattices containing the band insulator LaAlO3 and the correlated metal LaNiO3. Besides a suppression of holes at the apical oxygen, a central feature is the asymmetric response to strain in single unit cell superlattices: For tensile strain a band gap opens due to charge disproportionation at the Ni sites with two distinct magnetic moments of 1.45µB and 0.71µB. Under compressive stain, charge disproportionation is nearly quenched and the band gap collapses due to overlap of d 3z 2 −r 2 bands through a semimetallic state. This asymmetry in the electronic behavior is associated with the difference in octahedral distortions and rotations under tensile and compressive strain. The ligand hole density and the metallic state are quickly restored with increasing thickness of the (LaAlO3)n/(LaNiO3)n superlattice from n = 1 to n = 3.

Emergent long-range magnetic order in ultrathin (111)-oriented LaNiO3 films

npj Quantum Materials

The emergence of ferromagnetism in materials where the bulk phase does not show any magnetic order demonstrates that atomically precise films can stabilize distinct ground states and expands the phase space for the discovery of materials. Here, the emergence of long-range magnetic order is reported in ultrathin (111) LaNiO3 (LNO) films, where bulk LNO is paramagnetic, and the origins of this phase are explained. Transport and structural studies of LNO(111) films indicate that NiO6 octahedral distortions stabilize a magnetic insulating phase at the film/substrate interface and result in a thickness-dependent metal–insulator transition at t = 8 unit cells. Away from this interface, distortions relax and bulk-like conduction is regained. Synchrotron x-ray diffraction and dynamical x-ray diffraction simulations confirm a corresponding out-of-plane unit-cell expansion at the interface of all films. X-ray absorption spectroscopy reveals that distortion stabilizes an increased concentratio...

Effect of polar discontinuity on the growth of LaNiO[sub 3]/LaAlO[sub 3] superlattices

Applied Physics Letters, 2010

We have conducted a detailed microscopic investigation of [LaNiO3(1 u.c.)/LaAlO3(1 u.c.)]N superlattices grown on (001) SrTiO3 and LaAlO3 to explore the influence of polar mismatch on the resulting electronic and structural properties. Our data demonstrate that the initial growth on the non-polar SrTiO3 surface leads to a rough morphology and unusual 2+ valence of Ni in the first LaNiO3 layer, which is not observed after growth on the polar surface of LaAlO3. A newly devised model suggests that the polar mismatch can be resolved if the perovskite layers grow with an excess of LaO, which also accounts for the observed electronic, chemical, and structural effects.

Ab initio many-body GW correlations in the electronic structure of LaNiO2

Physical Review B, 2020

We present an ab initio GW self-energy calculation of the electronic structure of LaNiO2. With respect to density-functional theory we find that in GW the La 4f states undergo an important +2 eV upward shift from the Fermi level, while the O 2p states are pulled down by −1.5 eV, thus reinforcing the charge-transfer character of this material. However, GW many-body effects leave the d-like bands at the Fermi level almost unaffected, so that the Fermi-surface topology is preserved, unlike in cuprates.

Strain-controlled band engineering and self-doping in ultrathin LaNiO_{3} films

Physical Review B, 2012

We report on a systematic study of the temperature-dependent Hall coefficient and thermoelectric power in ultra-thin metallic LaNiO3 films that reveal a strain-induced, self-doping carrier transition that is inaccessible in the bulk. As the film strain varies from compressive to tensile at fixed composition and stoichiometry, the transport coefficients evolve in a manner strikingly similar to those of bulk hole-doped superconducting cuprates with varying doping level. Density functional calculations reveal that the strain-induced changes in the transport properties are due to self-doping in the low-energy electronic band structure. The results imply that thin-film epitaxy can serve as a new means to achieve hole-doping in other (negative) charge-transfer gap transition metal oxides without resorting to chemical substitution.

Loading...

Loading Preview

Sorry, preview is currently unavailable. You can download the paper by clicking the button above.