M. Kareev

Asymmetric orbital-lattice interactions in ultrathin correlated oxide films

Using resonant x-ray spectroscopies combined with density functional calculations, we find an asymmetric biaxial strain-induced d-orbital response in ultrathin films of the correlated metal LaNiO3 which are not accessible in the bulk. The sign of the misfit strain governs the stability of an octahedral breathing distortion, which, in turn, produces an emergent charge-ordered ground state with an altered ligand-hole density and bond covalency. Control of this new mechanism opens a pathway to rational orbital engineering, providing a platform for artificially designed Mott materials.

Strain-mediated metal-insulator transition in epitaxial ultrathin films of NdNiO3

We have synthesized epitaxial NdNiO3 ultrathin films in a layer-by-layer growth mode under tensile and compressive strain on SrTiO3 (001) and LaAlO3 (001), respectively. A combination of x-ray diffraction, temperature dependent resistivity, and soft x-ray absorption spectroscopy has been applied to elucidate electronic and structural properties of the samples. In contrast to the bulk NdNiO3, the metal-insulator transition under compressive strain is found to be completely quenched, while the transition remains under the tensile strain albeit modified from the bulk behavior.

Visualizing short-range charge transfer at the interfaces between ferromagnetic and superconducting oxides

The interplay between antagonistic superconductivity and ferromagnetism has been a interesting playground to explore the interaction between competing ground states. Although this effect in systems of conventional superconductors is better understood, the framework of the proximity effect at complex-oxide-based superconductor/ferromagnet interfaces is not so clear. The main difficulty originates from the lack of experimental tools capable of probing the interfaces directly with high spatial resolution. Here we harness cross-sectional scanning tunnelling microscopy and spectroscopy together with atomic-resolution electron microscopy to understand the buried interfaces between cuprate and manganite layers. The results show that the fundamental length scale of the electronic evolution between YBa2Cu3O(7-δ) (YBCO) and La2/3Ca1/3MnO3 (LCMO) is confined to the subnanometre range. Our findings provide a complete and direct microscopic picture of the electronic transition across the YBCO/LCMO interfaces, which is an important step towards understanding the competition between ferromagnetism and superconductivity in complex-oxide heterostructures.

Orbital control in strained ultra-thin LaNiO3/LaAlO3 superlattices

In pursuit of rational control of orbital polarization, we present a combined experimental and theoretical study of single-unit-cell superlattices of the correlated metal LaNiO3 and the band insulator LaAlO3. Polarized X-ray absorption spectra show a distinct asymmetry in the orbital response under strain. A splitting of orbital energies consistent with octahedral distortions is found for the case of compressive strain. In sharp contrast, for tensile strain, no splitting is found although a strong orbital polarization is present. Density functional theory calculations including a Hubbard U-term reveal that this asymmetry is a result of the interplay of strain and confinement that induces octahedral rotations and distortions and altered covalency in the bonding across the interfacial Ni-O-Al apical oxygen, leading to a charge disproportionation at the Ni sites for tensile strain.

Effect of polar discontinuity on the growth of LaNiO3/LaAlO3 superlattices

We have conducted a detailed microscopic investigation of [LaNiO3(1u2002u.c.)/LaAlO3(1u2002u.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 nonpolar SrTiO3 surface leads to a rough morphology and unusual 2+ valence of Ni in the initial LaNiO3 layer, which is not observed after growth on the polar surface of LaAlO3. A 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.

Strain-controlled band engineering and self-doping in ultrathin LaNiO 3 films

We report on a systematic study of the temperature-dependent Hall coefficient and thermoelectric power in ultra-thin metallic LaNiO

Sub-monolayer nucleation and growth of complex oxides at high supersaturation and rapid flux modulation

_3

Strain-dependent transport properties of the ultra-thin correlated metal, 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.

Metallic Conductance at the Interface of Tri-color Titanate Superlattices

We report on the non-trivial nanoscale kinetics of the deposition of novel complex oxide heterostructures composed of a unit-cell thick correlated metal LaNiO3 and dielectric LaAlO3. The multilayers demonstrate exceptionally good crystallinity and surface morphology maintained over the large number of layers, as confirmed by AFM, RHEED, and synchrotron X-ray diffraction. To elucidate the physics behind the growth, the temperature of the substrate and the deposition rate were varied over a wide range and the results were treated in the framework of a two-layer model. These results are of fundamental importance for synthesis of new phases of complex oxide heterostructures.

Ramp-Reversal Memory and Phase-Boundary Scarring in Transition Metal Oxides

We explore the electrical transport and magneto-conductance (MC) in quasi-two-dimensional strongly correlated ultra-thin films of LaNiO3 (LNO) to investigate the effect of hetero-epitaxial strain on electron?electron and electron?lattice interactions from the low to intermediate temperature range (2?170?K). The fully epitaxial 10 unit cell thick films spanning tensile strain up to ~4% are used to investigate the effects of enhanced carrier localization driven by a combination of weak localization (WL) and electron?electron interactions at low temperatures. The MC data show the importance of the increased contribution of WL to low-temperature quantum corrections. The obtained results demonstrate that with increasing tensile strain and reduced temperature, the quantum-confined LNO system gradually evolves from the Mott into the Mott?Anderson regime.