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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.

 

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.

 

Utilizing the powerful combination of molecular-beam epitaxy (MBE) and angle-resolved photoemission spectroscopy (ARPES), we produce and study the effect of different terminating layers on the electronic structure of the metallic delafossite PdCoO 2 . Attempts to introduce unpaired electrons and synthesize new antiferromagnetic metals akin to the isostructural compound PdCrO 2 have been made by replacing cobalt with iron in PdCoO 2 films grown by MBE. Using ARPES, we observe similar bulk bands in these PdCoO 2 films with Pd-, CoO 2 -, and FeO 2 -termination. Nevertheless, Pd- and CoO 2 -terminated films show a reduced intensity of surface states. Additionally, we are able to epitaxially stabilize PdFe x Co 1− x O 2 films that show an anomaly in the derivative of the electrical resistance with respect to temperature at 20 K, but do not display pronounced magnetic order. 

Functional properties of transition-metal oxides strongly depend on crystallographic defects; crystallographic lattice deviations can affect ionic diffusion and adsorbate binding energies. Scanning x-ray nanodiffraction enables imaging of local structural distortions across an extended spatial region of thin samples. Yet, localized lattice distortions remain challenging to detect and localize using nanodiffraction, due to their weak diffuse scattering. Here, we apply an unsupervised machine learning clustering algorithm to isolate the low-intensity diffuse scattering in as-grown and alkaline-treated thin epitaxially strained SrIrO3 films. We pinpoint the defect locations, find additional strain variation in the morphology of electrochemically cycled SrIrO3, and interpret the defect type by analyzing the diffraction profile through clustering. Our findings demonstrate the use of a machine learning clustering algorithm for identifying and characterizing hard-to-find crystallographic defects in thin films of electrocatalysts and highlight the potential to study electrochemical reactions at defect sites in operando experiments.

 

The unconventional superconductivity in Sr 2 RuO 4 is infamously susceptible to suppression by small levels of disorder such that it has been most commonly studied in extremely high-purity bulk crystals. Here, we harness local structural and spectroscopic scanning transmission electron microscopy measurements in epitaxial thin films of Sr 2 RuO 4 to disentangle the impact of different types of crystalline disorder on superconductivity. We find that cation off-stoichiometry during growth gives rise to two distinct types of disorder: mixed-phase structural inclusions that accommodate excess ruthenium and ruthenium vacancies when the growth is ruthenium-deficient. Several superconducting films host mixed-phase intergrowths, suggesting this microstructural disorder has relatively little impact on superconductivity. In a non-superconducting film, on the other hand, we measure a high density of ruthenium-vacancies [Formula: see text] with no significant reduction in the crystallinity of the film. The results suggest that ruthenium vacancy disorder, which is hidden to many structural probes, plays an important role in suppressing superconductivity. We discuss the broader implications of our findings to guide the future synthesis of this and other layered systems. 

Transition metal dichalcogenide heterostructures show strong interactions and can imprint a moiré potential to a separate layer. 

Tomographic spectroscopy reveals how the properties of topological materials can be engineered at interfaces.