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The effect of an electric field on local domain structure near a 24° tilt grain boundary in a 200 nm-thick Pb(Zr_0.2Ti_0.8)O₃bi-crystal ferroelectric film was probed using synchrotron nanodiffraction. The bi-crystal film was grown epitaxially on SrRuO₃-coated (001) SrTiO₃24° tilt bi-crystal substrates. From the nanodiffraction data, real-space maps of the ferroelectric domain structure around the grain boundary prior to and during application of a 200 kV cm⁻¹electric field were reconstructed. In the vicinity of the tilt grain boundary, the distributions of densities ofc-type tetragonal domains with thecaxis aligned with the film normal were calculated on the basis of diffracted intensity ratios ofc- anda-type domains and reference powder diffraction data. Diffracted intensity was averaged along the grain boundary, and it was shown that the density ofc-type tetragonal domains dropped to ∼50% of that of the bulk of the film over a range ±150 nm from the grain boundary. This work complements previous results acquired by band excitation piezoresponse force microscopy, suggesting that reduced nonlinear piezoelectric response around grain boundaries may be related to the change in domain structure, as well as to the possibility of increased pinning of domain wall motion. The implications of the results and analysis in terms of understanding the role of grain boundaries in affecting the nonlinear piezoelectric and dielectric responses of ferroelectric materials are discussed. 

Abstract Single-crystalline nickel-rich cathodes are a rising candidate with great potential for high-energy lithium-ion batteries due to their superior structural and chemical robustness in comparison with polycrystalline counterparts. Within the single-crystalline cathode materials, the lattice strain and defects have significant impacts on the intercalation chemistry and, therefore, play a key role in determining the macroscopic electrochemical performance. Guided by our predictive theoretical model, we have systematically evaluated the effectiveness of regaining lost capacity by modulating the lattice deformation via an energy-efficient thermal treatment at different chemical states. We demonstrate that the lattice structure recoverability is highly dependent on both the cathode composition and the state of charge, providing clues to relieving the fatigued cathode crystal for sustainable lithium-ion batteries. 

Abstract Lithium‐ion batteries are indispensable power sources for a wide range of modern electronic devices. However, battery lifespan remains a critical limitation, directly affecting the sustainability and user experience. Conventional battery failure analysis in controlled lab settings may not capture the complex interactions and environmental factors encountered in real‐world, in‐device operating conditions. This study analyzes the failure of commercial wireless earbud batteries as a model system within their intended usage context. Through multiscale and multimodal characterizations, the degradations from the material level to the device level are correlated, elucidating a failure pattern that is closely tied to the specific device configuration and operating conditions. The findings indicate that the ultimate failure mode is determined by the interplay of battery materials, cell structural design, and the in‐device microenvironment, such as temperature gradients and their fluctuations. This holistic, in‐device perspective on environmental influences provides critical insights for battery integration design, enhancing the reliability of modern electronics. 

Thin-film solid-state interfacial dealloying (thin-film SSID) is an emerging technique to design nanoarchitecture thin films. The resulting controllable 3D bicontinuous nanostructure is promising for a range of applications including catalysis, sensing, and energy storage. Using a multiscale microscopy approach, we combine X-ray and electron nano-tomography to demonstrate that besides dense bicontinuous nanocomposites, thin-film SSID can create a very fine (5–15 nm) nanoporous structure. Not only is such a fine feature among one of the finest fabrications by metal-agent dealloying, but a multilayer thin-film design enables creating nanoporous films on a wider range of substrates for functional applications. Through multimodal synchrotron diffraction and spectroscopy analysis with which the materials’ chemical and structural evolution in this novel approach is characterized in details, we further deduce that the contribution of change in entropy should be considered to explain the phase evolution in metal-agent dealloying, in addition to the commonly used enthalpy term in prior studies. The discussion is an important step leading towards better explaining the underlying design principles for controllable 3D nanoarchitecture, as well as exploring a wider range of elemental and substrate selections for new applications. 

The ever-increasing brightness of synchrotron radiation sources demands improved X-ray optics to utilize their capability for imaging and probing biological cells, nano-devices and functional matter on the nanometre scale with chemical sensitivity. Hard X-rays are ideal for high-resolution imaging and spectroscopic applications owing to their short wavelength, high penetrating power and chemical sensitivity. The penetrating power that makes X-rays useful for imaging also makes focusing them technologically challenging. Recent developments in layer deposition techniques have enabled the fabrication of a series of highly focusing X-ray lenses, known as wedged multi-layer Laue lenses. Improvements to the lens design and fabrication technique demand an accurate, robust,in situand at-wavelength characterization method. To this end, a modified form of the speckle tracking wavefront metrology method has been developed. The ptychographic X-ray speckle tracking method is capable of operating with highly divergent wavefields. A useful by-product of this method is that it also provides high-resolution and aberration-free projection images of extended specimens. Three separate experiments using this method are reported, where the ray path angles have been resolved to within 4 nrad with an imaging resolution of 45 nm (full period). This method does not require a high degree of coherence, making it suitable for laboratory-based X-ray sources. Likewise, it is robust to errors in the registered sample positions, making it suitable for X-ray free-electron laser facilities, where beam-pointing fluctuations can be problematic for wavefront metrology. 

Bicontinuous-nanostructured materials with a three-dimensionally (3D) interconnected morphology offer unique properties and potential applications in catalysis, biomedical sensing and energy storage. The new approach of solid-state interfacial dealloying (SSID) opens a route for fabricating bi-continuous metal–metal composites and porous metals at nano-/meso-scales via a self-organizing process driven by minimizing the system's free energy. Integrating SSID and thin film processing fully can open up a wide range of technological opportunities in designing novel functional materials; to-date, no experimental evidence has shown that 3D bi-continuous films can be formed with SSID, owing to the complexity of the kinetic mechanisms in thin film geometry and at nano-scales, despite the simple processing strategy in SSID. Here, we demonstrate that a fully-interconnected 3D bi-continuous structure can be achieved by this new approach, thin-film-SSID, using Fe–Ni film dealloyed by Mg film. The formation of a Fe–Mg x Ni bi-continuous 3D nano-structure was visualized and characterized via a multi-scale, multi-modal approach, combining electron transmission microscopy with synchrotron X-ray fluorescence nano-tomography and absorption spectroscopy. Phenomena involved with structural formation are discussed. These include surface dewetting, nano-size void formation among metallic ligaments, and interaction with a substrate. This work sheds light on the mechanisms of the SSID process, and sets a path for manufacturing of thin-film materials for future nano-structured metallic materials.