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Epitaxial untwinned SrRuO3 thin films were grown on (110)-oriented DyScO3 substrates by molecular-beam epitaxy. We report an exceptional sample with a residual resistivity ratio (RRR), ρ [300 K]/ρ [4 K] of 205 and a ferromagnetic Curie temperature, TC, of 168.3 K. We compare the properties of this sample to other SrRuO3 films grown on DyScO3(110) with RRRs ranging from 8.8 to 205, and also compare it to the best reported bulk single crystal of SrRuO3. We determine that SrRuO3 thin films grown on DyScO3(110) have an enhanced TC as long as the RRR of the thin film is above a minimum electrical quality threshold. This RRR threshold is about 20 for SrRuO3. Films with lower RRR exhibit TCs that are significantly depressed from the intrinsic strain-enhanced value.

 

Molecular-beam epitaxy enables ultrathin functional materials to be combined in heterostructures to create emergent phenomena at the interface. Magnetic skyrmions are an example of an exciting phase found in such heterostructures. SrRuO3 and SrRuO3-based heterostructures have been at the center of the debate on whether a hump-like feature appearing in Hall resistivities is sufficient evidence to prove the presence of skyrmions in a material. To address the ambiguity, we synthesize a model heterostructure with engineered Berry curvature that combines, in parallel, a positive anomalous Hall effect (AHE) channel (a Sr0.6Ca0.4RuO3 layer) with a negative AHE channel (a SrRuO3 layer). We demonstrate that the two opposite AHE channels can be combined to artificially reproduce a “hump-like” feature, which closely resembles the hump-like feature typically attributed to the topological Hall effect and the presence of chiral spin textures, such as skyrmions. We compare our heterostructure with a parallel resistor model, where the inputs are the AHE data from individual Sr0.6Ca0.4RuO3 and SrRuO3 films. To check for the presence of skyrmions, we measure the current dependence, angle dependence, and minor loop dependence of Rhump in the heterostructure. Despite the clear hump, no evidence of skyrmions is found.

 

The concept of remote epitaxy involves a two-dimensional van der Waals layer covering the substrate surface, which still enable adatoms to follow the atomic motif of the underlying substrate. The mode of growth must be carefully defined as defects, e.g., pinholes, in two-dimensional materials can allow direct epitaxy from the substrate, which, in combination with lateral epitaxial overgrowth, could also form an epilayer. Here, we show several unique cases that can only be observed for remote epitaxy, distinguishable from other two-dimensional material-based epitaxy mechanisms. We first grow BaTiO₃on patterned graphene to establish a condition for minimizing epitaxial lateral overgrowth. By observing entire nanometer-scale nuclei grown aligned to the substrate on pinhole-free graphene confirmed by high-resolution scanning transmission electron microscopy, we visually confirm that remote epitaxy is operative at the atomic scale. Macroscopically, we also show variations in the density of GaN microcrystal arrays that depend on the ionicity of substrates and the number of graphene layers.

 

Strain-engineering is a powerful means to tune the polar, structural, and electronic instabilities of incipient ferroelectrics. KTaO3 is near a polar instability and shows anisotropic superconductivity in electron-doped samples. Here, we demonstrate growth of high-quality KTaO3 thin films by molecular-beam epitaxy. Tantalum was provided by either a suboxide source emanating a TaO2 flux from Ta2O5 contained in a conventional effusion cell or an electron-beam-heated tantalum source. Excess potassium and a combination of ozone and oxygen (10% O3 + 90% O2) were simultaneously supplied with the TaO2 (or tantalum) molecular beams to grow the KTaO3 films. Laue fringes suggest that the films are smooth with an abrupt film/substrate interface. Cross-sectional scanning transmission electron microscopy does not show any extended defects and confirms that the films have an atomically abrupt interface with the substrate. Atomic force microscopy reveals atomic steps at the surface of the grown films. Reciprocal space mapping demonstrates that the films, when sufficiently thin, are coherently strained to the SrTiO3 (001) and GdScO3 (110) substrates. 

New properties and exotic quantum phenomena can form due to periodic nanotextures, including Moire patterns, ferroic domains, and topologically protected magnetization and polarization textures. Despite the availability of powerful tools to characterize the atomic crystal structure, the visualization of nanoscale strain-modulated structural motifs remains challenging. Here, we develop nondestructive real-space imaging of periodic lattice distortions in thin epitaxial films and report an emergent periodic nanotexture in a Mott insulator. Specifically, we combine iterative phase retrieval with unsupervised machine learning to invert the diffuse scattering pattern from conventional X-ray reciprocal-space maps into real-space images of crystalline displacements. Our imaging in PbTiO₃/SrTiO₃superlattices exhibiting checkerboard strain modulation substantiates published phase-field model calculations. Furthermore, the imaging of biaxially strained Mott insulator Ca₂RuO₄reveals a strain-induced nanotexture comprised of nanometer-thin metallic-structure wires separated by nanometer-thin Mott-insulating-structure walls, as confirmed by cryogenic scanning transmission electron microscopy (cryo-STEM). The nanotexture in Ca₂RuO₄film is induced by the metal-to-insulator transition and has not been reported in bulk crystals. We expect the phasing of diffuse X-ray scattering from thin crystalline films in combination with cryo-STEM to open a powerful avenue for discovering, visualizing, and quantifying the periodic strain-modulated structures in quantum materials.

 

Strain-engineering is a powerful means to tune the polar, structural, and electronic instabilities of incipient ferroelectrics. KTaO 3 is near a polar instability and shows anisotropic superconductivity in electron-doped samples. Here, we demonstrate growth of high-quality KTaO 3 thin films by molecular-beam epitaxy. Tantalum was provided by either a suboxide source emanating a TaO 2 flux from Ta 2 O 5 contained in a conventional effusion cell or an electron-beam-heated tantalum source. Excess potassium and a combination of ozone and oxygen (10% O 3 + 90% O 2 ) were simultaneously supplied with the TaO 2 (or tantalum) molecular beams to grow the KTaO 3 films. Laue fringes suggest that the films are smooth with an abrupt film/substrate interface. Cross-sectional scanning transmission electron microscopy does not show any extended defects and confirms that the films have an atomically abrupt interface with the substrate. Atomic force microscopy reveals atomic steps at the surface of the grown films. Reciprocal space mapping demonstrates that the films, when sufficiently thin, are coherently strained to the SrTiO 3 (001) and GdScO 3 (110) substrates.