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The discovery of superconductivity in infinite-layer nickelates has sparked great interest due to their potential analogy with the unconventional cuprate superconductors. However, investigations of this system have been limited by the challenges in materials control and synthesis driven by substantial thermodynamic instability, making it difficult to reach an experimental consensus. Hence, establishing a robust synthetic route to highly crystalline infinite-layer nickelates is of paramount importance. Here, we present and discuss recent progress on the reproducible two-step synthesis of (Nd,Sr)NiO2 via the stabilization of high-quality perovskite nickelates and the subsequent topotactic transition to the infinite-layer phase. In particular, we discuss the important factors, such as cation stoichiometry and epitaxial strain, which significantly impact the crystallinity of both phases, accompanied by careful structural characterization. These results on robust synthesis can help accelerate the experimental investigation of the intrinsic physical properties of these complex strongly correlated materials.more » « less
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Mechanical strain presents an effective control over symmetry-breaking phase transitions. In quantum paralelectric SrTiO3, strain can induce ferroelectric order via modification of the local Ti potential energy landscape. However, brittle bulk materials can only withstand limited strain range (~0.1%). Taking advantage of nanoscopically-thin freestanding membranes, we demonstrate an in-situ strain-induced reversible ferroelectric transition in freestanding SrTiO3 membranes. We measure the ferroelectric order by detecting the local anisotropy of the Ti 3d orbital signature using x-ray linear dichroism at the Ti-K pre-edge, while the strain is determined by x-ray diffraction. With reduced thickness, the SrTiO3 membranes remain elastic with >1% tensile strain cycles. A robust displacive ferroelectricity appears beyond a temperature-dependent critical strain. Interestingly, we discover a crossover from a classical ferroelectric transition to a quantum regime at low temperatures, which enhances strain-induced ferroelectricity. Our results offer new opportunities to strain engineer functional properties in low dimensional quantum materials and provide new insights into the role of ferroelectric fluctuations in quantum paraelectric SrTiO3.more » « less
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Abstract Antiferroelectrics are a promising class of materials for applications in capacitive energy storage and multi‐state memory, but comprehensive control of their functional properties requires further research. In thin films, epitaxial strain and size effects are important tuning knobs but difficult to probe simultaneously due to low critical thicknesses of common lead‐based antiferroelectrics. Antiferroelectric NaNbO3enables opportunities for studying size effects under strain, but electrical properties of ultra‐thin films have not been thoroughly investigated due to materials challenges. Here, high‐quality, epitaxial, coherently‐strained NaNbO3films are synthesized from 35‐ to 250‐ nm thickness, revealing a transition from a fully ferroelectric state to coexisting ferroelectric and antiferroelectric phases with increasing thickness. The electrical performance of this phase coexistence is analyzed through positive‐up negative‐down and first‐order reversal curve measurements. Further increasing thickness leads to a fully ferroelectric state due to a strain relief mechanism that suppresses the antiferroelectricity. The potential of engineering competing ferroic orders in NaNbO3for multiple applications is evaluated, reporting significantly enhanced recoverable energy density (20.6 J cm−3at 35 nm) and energy efficiency (90% at 150 nm) relative to pure bulk NaNbO3as well as strong retention and fatigue performance with multiple accessible polarization states in the intermediate thickness films.more » « less
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Abstract Recent theoretical studies have suggested that transition metal perovskite oxide membranes can enable surface phonon polaritons in the infrared range with low loss and much stronger subwavelength confinement than bulk crystals. Such modes, however, have not been experimentally observed so far. Here, using a combination of far-field Fourier-transform infrared (FTIR) spectroscopy and near-field synchrotron infrared nanospectroscopy (SINS) imaging, we study the phonon polaritons in a 100 nm thick freestanding crystalline membrane of SrTiO3transferred on metallic and dielectric substrates. We observe a symmetric-antisymmetric mode splitting giving rise to epsilon-near-zero and Berreman modes as well as highly confined (by a factor of 10) propagating phonon polaritons, both of which result from the deep-subwavelength thickness of the membranes. Theoretical modeling based on the analytical finite-dipole model and numerical finite-difference methods fully corroborate the experimental results. Our work reveals the potential of oxide membranes as a promising platform for infrared photonics and polaritonics.more » « less
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