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            Pattern formation in spin systems with continuous-rotational symmetry (CRS) provides a powerful platform to study emergent complex magnetic phases and topological defects in condensed-matter physics. However, its understanding and correlation with unconventional magnetic order along with high-resolution nanoscale imaging are challenging. Here, we employ scanning nitrogen vacancy (NV) magnetometry to unveil the morphogenesis of spin cycloids at both the local and global scales within a single ferroelectric domain of (111)-oriented BiFeO3, which is a noncollinear antiferromagnet, resulting in formation of a glassy labyrinthine pattern. We find that the domains of locally oriented cycloids are interconnected by an array of topological defects and exhibit isotropic energy landscape predicted by first-principles calculations. We propose that the CRS of spin-cycloid propagation directions within the (111) drives the formation of the labyrinthine pattern and the associated topological defects such as antiferromagnetic skyrmions. Unexpectedly, reversing the as-grown ferroelectric polarization from [ ] to [111] produces a noncycloidal NV image contrast which could be attributed to either the emergence of a uniformly magnetized state or a reversal of the cycloid polarity. These findings highlight that (111)-oriented BiFeO3is not only important for studying the fascinating subject of pattern formation but could also be utilized as an ideal platform for integrating novel topological defects in the field of antiferromagnetic spintronics.more » « lessFree, publicly-accessible full text available April 29, 2026
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            Abstract Bismuth ferrite has garnered considerable attention as a promising candidate for magnetoelectric spin-orbit coupled logic-in-memory. As model systems, epitaxial BiFeO3thin films have typically been deposited at relatively high temperatures (650–800 °C), higher than allowed for direct integration with silicon-CMOS platforms. Here, we circumvent this problem by growing lanthanum-substituted BiFeO3at 450 °C (which is reasonably compatible with silicon-CMOS integration) on epitaxial BaPb0.75Bi0.25O3electrodes. Notwithstanding the large lattice mismatch between the La-BiFeO3, BaPb0.75Bi0.25O3, and SrTiO3(001) substrates, all the layers in the heterostructures are well ordered with a [001] texture. Polarization mapping using atomic resolution STEM imaging and vector mapping established the short-range polarization ordering in the low temperature grown La-BiFeO3. Current-voltage, pulsed-switching, fatigue, and retention measurements follow the characteristic behavior of high-temperature grown La-BiFeO3, where SrRuO3typically serves as the metallic electrode. These results provide a possible route for realizing epitaxial multiferroics on complex-oxide buffer layers at low temperatures and opens the door for potential silicon-CMOS integration.more » « less
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            Abstract The pursuit of smaller, energy‐efficient devices drives the exploration of electromechanically active thin films (<1 µm) to enable micro‐ and nano‐electromechanical systems. While the electromechanical response of such films is limited by substrate‐induced mechanical clamping, large electromechanical responses in antiferroelectric and multilayer thin‐film heterostructures have garnered interest. Here, multilayer thin‐film heterostructures based on antiferroelectric PbHfO3and ferroelectric PbHf1‐xTixO3overcome substrate clamping to produce electromechanical strains >4.5%. By varying the chemistry of the PbHf1‐xTixO3layer (x = 0.3‐0.6) it is possible to alter the threshold field for the antiferroelectric‐to‐ferroelectric phase transition, reducing the field required to induce the onset of large electromechanical response. Furthermore, varying the interface density (from 0.008 to 3.1 nm−1) enhances the electrical‐breakdown field by >450%. Attaining the electromechanical strains does not necessitate creating a new material with unprecedented piezoelectric coefficients, but developing heterostructures capable of withstanding large fields, thus addressing traditional limitations of thin‐film piezoelectrics.more » « less
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            Abstract The dielectric gap between the scanning probe microscopy (SPM) tip and the surface of a ferroelectric using conductive atomic force microscopy and piezoresponse force microscopy (PFM) is investigated. While the gap functions as a dielectric layer, it also allows tunneling current to inject charges into the ferroelectric when a critical loading force between 10–20 µN is applied to a tip with a radius of 25 nm under a bias voltage of 0.5 V. It is observed that the permittivity of the dielectric gap determines the coercive voltage measured by the piezoresponse hysteresis loop. While such studies done in air often produce coercive voltages much larger than those studied for the same materials in capacitor‐based studies, the use of high permittivity media such as water (ɛr= 79) or silicone oil (ɛr= 2.1‐2.8) produces coercive fields that more closely match those measured in conventional capacitor‐based polarization hysteresis loop measurements. Furthermore, using water as a dielectric medium in PFM imaging enhances the accuracy in extracting the amplitude and phase data from periodically poled lithium niobate crystals. These findings provide insight into the nanoscale phenomena of polarization switching instigated by the SPM tip and provide a pathway to improved quantitative studies.more » « less
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            Abstract The Rashba effect enables control over the spin degree of freedom, particularly in polar materials where the polar symmetry couples to Rashba‐type spin splitting. The exploration of this effect, however, has been hindered by the scarcity of polar materials exhibiting the bulk‐Rashba effect and rapid spin‐relaxation effects dictated by the D'yakonov–Perel mechanism. Here, a polar LiNbO3‐typeR3cphase of Bi1‐xIn1+xO3withx≈0.15–0.24 is stabilized via epitaxial growth, which exhibits a bulk‐Rashba effect with suppressed spin relaxation as a result of its unidirectional spin texture. As compared to the previously observed non‐polarPnmaphase, this polar phase exhibits higher conductivity, reduced bandgap, and enhanced dielectric and piezoelectric responses. Combining first‐principles calculations and multimodal magnetotransport measurements, which reveal weak (anti)localization, anisotropic magnetoresistance, planar‐Hall effect, and nonreciprocal charge transport, a bulk‐Rashba effect without rapid spin relaxation is demonstrated. These findings offer insights into spin‐orbit coupling physics within polar oxides and suggest potential spintronic applications.more » « less
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