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Register a new userControlling the electronic interface properties of AlO$_x$/SrTiO$_3$ heterostructures
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Depositing disordered Al on top of SrTiO$_3$ is a cheap and easy way to create a two-dimensional electron system in the SrTiO$_3$ surface layers. To facilitate future device applications we passivate the heterostructure by a disordered LaAlO$_3$ capping layer to study the electronic properties by complementary x-ray photoemission spectroscopy and transport measurements on the very same samples. We also tune the electronic interface properties by adjusting the oxygen pressure during film growth.
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We have studied the chemical and electronic properties of LaAlO3/SrVO3 ultrathin films by combining hard x-ray photoemission spectroscopy and transport measurements. We compare single SrVO3 (SVO) ultrathin films and SrVO3 buried below a polar LaAlO3 (LAO) thin layer, both epitaxially grown on SrTiO3. While ultrathin films (4 unit cells) of SVO do show insulating behavior over the entire temperature range, the LAO/SVO interface has a resistivity minimum at 250 K. When increasing the SVO layer thickness, the minimum is observed to shift to higher temperatures, but the resistivity stays always smaller than that of comparable SVO single films. Hard x-ray photoemission spectroscopy reveals a surface or interface related V5+ component in the V 2p spectra for SVO films and LAO/SVO heterostructures, respectively, attributed to a strongly oxidized component. This chemical reconstruction is weaker in LAO/SVO heterostructures compared to single SVO films. We show that this dead layer in SVO ultrathin films has to be considered when the film thickness reaches the few unit-cells limit and propose solutions on how to prevent this detrimental effect.
Epitaxial interfaces and superlattices comprised of polar and non-polar perovskite oxides have generated considerable interest because they possess a range of desirable properties for functional devices. In this work, emergent polarization in superlattices of SrTiO$_3$ (STO) and LaCrO$_3$ (LCO) is demonstrated. By controlling the interfaces between polar LCO and non-polar STO, polarization is induced throughout the STO layers of the superlattice. Using x-ray absorption near-edge spectroscopy and aberration-corrected scanning transmission electron microscopy displacements of the Ti cations off-center within TiO6 octahedra along the superlattice growth direction are measured. This distortion gives rise to built-in potential gradients within the STO and LCO layers, as measured by in situ x-ray photoelectron spectroscopy. Density functional theory models explain the mechanisms underlying this behavior, revealing the existence of both an intrinsic polar distortion and a built-in electric field, which are due to alternately positively and negatively charged interfaces in the superlattice. This study paves the way for controllable polarization for carrier separation in multilayer materials and highlights the crucial role that interface structure plays in governing such behavior.
The transport and thermoelectric properties of the interface between SrTiO$_3$ and a 26-monolayer thick LaAlO$_3$-layer grown at high oxygen-pressure have been investigated at temperatures from 4.2 K to 100 K and in magnetic fields up to 18 T. For $T>$ 4.2 K, two different electron-like charge carriers originating from two electron channels which contribute to transport are observed. We probe the contributions of a degenerate and a non-degenerate band to the thermoelectric power and develop a consistent model to describe the temperature dependence of the thermoelectric tensor. Anomalies in the data point to an additional magnetic field dependent scattering.
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.
The effect of growth conditions on the structural and electronic properties of the polar/non-polar LaCrO$_3$/SrTiO$_3$ (LCO/STO) interface has been investigated. The interface is either insulating or metallic depending on growth conditions. A high sheet carrier concentration of 2x10$^{16}$ cm$^{-2}$ and mobility of 30,000 cm$^2$/V s is reported for the metallic interfaces, which is similar to the quasi-two dimensional gas at the LaAlO$_{3}$/SrTiO$_{3}$ interface with similar growth conditions. High-resolution synchrotron X-ray-based structural determination of the atomic-scale structures of both metallic and insulating LCO/STO interfaces show chemical intermixing and an interfacial lattice expansion. Angle resolved photoemission spectroscopy of 2 and 4 uc metallic LCO/STO shows no intensity near the Fermi level indicating that the conducting region is occurring deep enough in the substrate to be inaccessible to photoemission spectroscopy. Post-growth annealing in flowing oxygen causes a reduction in the sheet carrier concentration and mobility for the metallic interface while annealing the insulating interface at high temperatures and low oxygen partial pressures results in metallicity. These results highlight the critical role of defects related to oxygen vacancies on the creation of mobile charge carriers at the LCO/STO heterointerface.
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