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

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.Comment: 13 pages, 6 figure

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

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.Comment: 3 pages, 3 figure

Orbital control in strained ultra-thin LaNiO3_3/LaAlO3_3 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 LaNiO$_3$ and the band insulator LaAlO$_3$. 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 induces octahedral rotations and distortions and altered covalency in the bonding across the interfacial Ni-O-Al apical oxygen, leading to a charge disporportionation at the Ni sites for tensile strain.Comment: 4 pages. 5 figure

Epitaxial strain modulated electronic properties of interface controlled nickelate superlattice

Perovskite nickelate heterostructure consisting of single unit cell of EuNiO$_3$ and LaNiO$_3$ have been grown on a set of single crystalline substrates by pulsed laser interval deposition to investigate the effect of epitaxial strain on electronic and magnetic properties at the extreme interface limit. Despite the variation of substrate in-plane lattice constants and lattice symmetry, the structural response to heterostructuring is primarily controlled by the presence of EuNiO$_3$ layer. In sharp contrast to bulk LaNiO$_3$ or EuNiO$_3$, the superlattices grown under tensile strains exhibit metal to insulator transition (MIT) below room temperature. The onset of magnetic and electronic transitions associated with the MIT can be further separated by application of large tensile strain. Furthermore, these transitions can be entirely suppressed by very small compressive strain. X-ray resonant absorption spectroscopy measurements reveal that such strain-controlled MIT is directly linked to strain induced self-doping effect without any chemical doping.Comment: Accepted in Phys. Rev.

Strain-mediated metal-insulator transition in epitaxial ultra-thin films of NdNiO3

We have synthesized epitaxial NdNiO$_{3}$ ultra-thin films in a layer-by-layer growth mode under tensile and compressive strain on SrTiO$_{3}$ (001) and LaAlO$_3$ (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 NdNiO$_{3}$, 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.Comment: 4 pages, 4 figure