The authors report on the crystallographic orientation dependence of the Schottky properties for heterojunctions between a half-metallic ferromagnet La$_0.6$Sr$_0.4$MnO$_3$ (LSMO) and Nb-doped SrTiO3 semiconductor. The Schottky barrier height determined by in situ photoemission measurements is independent for the substrate orientations (001) and (110), while the magnetic properties of LSMO (110) films are more enhanced than for (001) films. These results suggest that the performance of magnetic devices based on ferromagnetic manganite is improved by using (110)-oriented substrates.
Thin film synthesis methods developed over the past decades have unlocked emergent interface properties ranging from conductivity to ferroelectricity. However, our attempts to exercise precise control over interfaces are constrained by a limited understanding of growth pathways and kinetics. Here we demonstrate that shuttered molecular beam epitaxy induces rearrangements of atomic planes at a polar / non-polar junction of LaFeO$_3$ (LFO) / $n$-SrTiO$_3$ (STO) depending on the substrate termination. Surface characterization confirms that substrates with two different (TiO$_2$ and SrO) terminations were prepared prior to LFO deposition; however, local electron energy loss spectroscopy measurements of the final heterojunctions show a predominantly LaO / TiO$_2$ interfacial junction in both cases. Ab initio simulations suggest that the interfaces can be stabilized by trapping extra oxygen (in LaO / TiO$_2$) and forming oxygen vacancies (in FeO$_2$ / SrO), which points to different growth kinetics in each case and may explain the apparent disappearance of the FeO$_2$ / SrO interface. We conclude that judicious control of deposition timescales can be used to modify growth pathways, opening new avenues to control the structure and properties of interfacial systems.
Charge transfer induced interfacial ferromagnetism and its impact on the exchange bias effect in La$_{0.7}$Sr$_{0.3}$MnO$_3$/NdNiO$_3$ correlated oxide heterostructures were investigated by soft x-ray absorption and x-ray magnetic circular dichroism spectra in a temperature range from 10 to 300 K. Besides the antiferromagnetic Ni$_3^+$ cations which are naturally part of the NdNiO$_3$ layer, Ni$_2^+$ ions are formed at the interface due to a charge transfer mechanism involving the Mn element of the adjacent layer. They exhibit a ferromagnetic behavior due to the exchange coupling to the Mn$_4^+$ ions in the La$_{0.7}$Sr$_{0.3}$MnO$_3$ layer. This can be seen as detrimental to the strength of the unidirectional anisotropy since a significant part of the interface does not contribute to the pinning of the ferromagnetic layer. By analyzing the line shape changes of the x-ray absorption at the Ni L$_{2,3}$ edges, the metal-insulator transition of the NdNiO$_3$ layer is resolved in an element specific manner. This phase transition is initiated at about 120 K, way above the paramagnetic to antiferromagnetic transition of NdNiO$_3$ layer which measured to be 50 K. Exchange bias and enhanced coercive fields were observed after field cooling the sample through the Neel temperature of the NdNiO$_3$ layer. Different from La$_{0.7}$Sr$_{0.3}$MnO$_3$/LaNiO$_3$, the exchange bias observed in La$_{0.7}$Sr$_{0.3}$MnO$_3$/NdNiO$_3$ is due to the antiferromagnetism of NdNiO$_3$ and the frustration at the interface. These results suggest that reducing the interfacial orbital hybridization may be used as a tunable parameter for the strength of the exchange bias effect in all-oxide heterostructures which exhibit a charge transfer mechanism.
Ionic crystals terminated at oppositely charged polar surfaces are inherently unstable and expected to undergo surface reconstructions to maintain electrostatic stability. Essentially, an electric field that arises between oppositely charged atomic planes gives rise to a built-in potential that diverges with thickness. In ultra thin film form however the polar crystals are expected to remain stable without necessitating surface reconstructions, yet the built-in potential has eluded observation. Here we present evidence of a built-in potential across polar lao ~thin films grown on sto ~substrates, a system well known for the electron gas that forms at the interface. By performing electron tunneling measurements between the electron gas and a metallic gate on lao ~we measure a built-in electric field across lao ~of 93 meV/AA. Additionally, capacitance measurements reveal the presence of an induced dipole moment near the interface in sto, illuminating a unique property of sto ~substrates. We forsee use of the ionic built-in potential as an additional tuning parameter in both existing and novel device architectures, especially as atomic control of oxide interfaces gains widespread momentum.
The magnetic dead layers in films a few nanometers thick are investigated for La$_{0.7}$Sr$_{0.3}$MnO$_3$ on (001)-oriented SrTiO$_3$ (STO), LaAlO$_3$ (LAO) and (LaAlO$_3$)$_{0.3}$(Sr$_2$TaAlO$_6$)$_{0.7}$ (LSAT) substrates. An anomalous moment found to persist above the Curie temperature of the La$_{0.7}$Sr$_{0.3}$MnO$_3$ films is not attributed to the films, but to oxygen vacancies at or near the surface of the substrate. The contribution to the moment from the substrate is as high as 20 $mu$B/nm$^2$ in the case of STO or LSAT. The effect is increased by adding an STO cap layer. Taking this d-zero magnetism into account, extrapolated magnetic dead layer thicknesses of 0.8 nm, 1.5 nm and 3.0 nm are found for the manganite films grown on LSAT, STO and LAO substrates, respectively. An STO cap layer eliminates the LSMO dead layer.
Hard x-ray photoelectron spectroscopy (HAXPES) and variable kinetic energy x-ray photoelectron spectroscopy (VKE-XPS) analyses have been performed on 10 unit cell La$_{(1-{delta})}$Al$_{(1+{delta})}$O$_3$ films, with La:Al ratios of 1.1, 1.0, and 0.9, deposited on SrTiO$_3$. Of the three films, only the Al-rich film was known to have a conductive interface. VKE-XPS, coupled with maximum entropy analysis, shows significant differences in the compositional depth profile between the Al-rich, the La-rich, and stoichiometric films; significant La enrichment at the interface is observed in the La-rich and stoichiometric films, while the Al-rich shows little to no intermixing. Additionally, the La-rich and stoichiometric films show a high concentration of Al at the surface, which is not observed in the Al-rich film. HAXPES valence band (VB) analysis shows a broadening of the VB for the Al-rich sample relative to the stoichiometric and La-rich samples, which have insulating interfaces. This broadening is consistent with an electric field across the Al-rich film. These results are consistent with a defect driven electronic reconstruction.