Perovskite SrIrO3 films and its heterostructures are very promising, yet less researched, avenues to explore interesting physics originating from the interplay between strong spin–orbit coupling and electron correlations. Elemental iridium is a commonly used source for molecular beam epitaxy (MBE) synthesis of SrIrO3 films. However, elemental iridium is extremely difficult to oxidize and evaporate while maintaining an ultra-high vacuum and a long mean free path. Here, we calculated a thermodynamic phase diagram to highlight these synthesis challenges for phase-pure SrIrO3 and other iridium-based oxides. We addressed these challenges using a novel solid-source metal-organic MBE approach that rests on the idea of modifying the metal-source chemistry. Phase-pure, single-crystalline, coherent, epitaxial (001)pc SrIrO3 films on (001) SrTiO3 substrate were grown. Films demonstrated semi-metallic behavior, Kondo scattering, and weak antilocalization. Our synthesis approach has the potential to facilitate research involving iridate heterostructures by enabling their atomically precise syntheses.
more »
« less
Detection of decoupled surface and bulk states in epitaxial orthorhombic SrIrO3 thin films
We report the experimental evidence of evolving lattice distortion in high quality epitaxial orthorhombic SrIrO3(001) thin films fully strained on (001) SrTiO3 substrates. Angle-resolved X-ray photoemission spectroscopy studies show that the surface layer of 5 nm SrIrO3 films is Sr–O terminated, and subsequent layers recover the semimetallic state, with the band structure consistent with an orthorhombic SrIrO3(001) having the lattice constant of the substrate. While there is no band folding in the experimental band structure, additional super-periodicity is evident in low energy electron diffraction measurements, suggesting the emergence of a transition layer with crystal symmetry evolving from the SrTiO3 substrate to the SrIrO3(001) surface. Our study sheds light on the misfit relaxation mechanism in epitaxial SrIrO3 thin films in the orthorhombic phase, which is metastable in bulk.
more »
« less
- Award ID(s):
- 1710461
- PAR ID:
- 10597318
- Publisher / Repository:
- American Institute of Physics
- Date Published:
- Journal Name:
- AIP Advances
- Volume:
- 10
- Issue:
- 4
- ISSN:
- 2158-3226
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Sb thin films have attracted wide interest due to their tunable band structure, topological phases, high electron mobility, and thermoelectric properties. We successfully grow epitaxial Sb thin films on a closely lattice-matched GaSb(001) surface by molecular beam epitaxy. We find a novel anisotropic directional dependence on their structural, morphological, and electronic properties. The origin of the anisotropic features is elucidated using first-principles density functional theory (DFT) calculations. The growth regime of crystalline and amorphous Sb thin films was determined by mapping the surface reconstruction phase diagram of the GaSb(001) surface under Sb2 flux, with confirmation of structural characterizations. Crystalline Sb thin films show a rhombohedral crystal structure along the rhombohedral (211) surface orientation parallel to the cubic (001) surface orientation of the GaSb substrate. At this coherent interface, Sb atoms are aligned with the GaSb lattice along the [1̄10] crystallographic direction but are not aligned well along the [110] crystallographic direction, which results in anisotropic features in reflection of high-energy electron diffraction patterns, misfit dislocation formation, surface morphology, and transport properties. Our DFT calculations show that the preferential orientation of the rhombohedral Sb (211) plane may originate from the GaSb surface, where Sb atoms align with the Ga and Sb atoms on the reconstructed surface. The formation energy calculations confirm the stability of the experimentally observed structures. Our results provide optimal film growth conditions for further studies of novel properties of Bi1−xSbx thin films with similar lattice parameters and an identical crystal structure, as well as functional heterostructures of them with III–V semiconductor layers along the (001) surface orientation, supported by a theoretical understanding of the anisotropic film orientation.more » « less
-
GdFe₀.₅Cr₀.₅O₃ (GFCO) is a single-phase magnetoelectric multiferroic at temperatures close to ambient. Epitaxial thin films of this orthorhombic perovskite would offer the possibility of tuning its electrical and magnetic properties through control of strain and interface effects. Here, 200 nm thick GFCO thin films have been grown on (001) SrTiO3 substrates by solution synthesis and the microstructures have been investigated by cross-sectional transmission electron microscopy. The GFCO films are epitaxial but exhibit a mixture of three different orientation relationships in the form of domains ≈50 nm in diameter. Geometric analyses of the lattice matching show that the misfits for these domains would be tensile with magnitudes of less than 2 %. Pockets of a SrCrO4 reaction product form at the film/substrate interface and do not exhibit any simple orientation with the adjacent phases. The product morphology indicates that the outward diffusion of Sr is more rapid than the inward diffusion of Cr, and this is related to the microstructures of the surrounding phases. These data show that epitaxial films of GFCO can be obtained via this route, but careful control of process parameters would be required to produce single-domain films, and alternate substrates or buffer layers would be needed to inhibit SrCrO4 formation.more » « less
-
The temperature-dependent layer-resolved structure of 3 to 44 unit cell thick SrRuO3 (SRO) films grown on Nb-doped SrTiO3 substrates is investigated using a combination of high-resolution synchrotron x-ray diffraction and high-resolution electron microscopy to understand the role that structural distortions play in suppressing ferromagnetism in ultra-thin SRO films. The oxygen octahedral tilts and rotations and Sr displacements characteristic of the bulk orthorhombic phase are found to be strongly dependent on temperature, the film thickness, and the distance away from the film–substrate interface. For thicknesses, t, above the critical thickness for ferromagnetism (t > 3 uc), the orthorhombic distortions decrease with increasing temperature above TC. Below TC, the structure of the films remains constant due to the magneto-structural coupling observed in bulk SRO. The orthorhombic distortions are found to be suppressed in the 2–3 interfacial layers due to structural coupling with the SrTiO3 substrate and correlate with the critical thickness for ferromagnetism in uncapped SRO films.more » « less
-
Dry oxidation of Si (001) beneath a thin epitaxial SrTiO3 layer has been studied using furnace annealing in flowing oxygen. A 10-nm layer of SrTiO3 is epitaxially grown on Si with no SiO2 interlayer. For such a structure, an annealing temperature of 800 °C was found to be the limiting temperature to prevent silicate formation and disruption of the interface structure. The effect of annealing time on the thickness of the SiO2 layer was investigated. In situ x-ray photoelectron spectroscopy and reflection-high-energy electron diffraction were used to ensure that the quality of SrTiO3 is unchanged after the annealing process. The experimental annealing data are compared with a theoretical oxygen diffusion model based on that of Deal, Grove, and Massoud. The model fits the experimental data well, indicating that oxygen diffusion through the SrTiO3 layer is not the limiting factor. One can therefore readily control the thickness of the SiO2 interlayer by simply controlling the annealing time in flowing oxygen.more » « less
An official website of the United States government
