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While intensive efforts have been devoted to studying the nature of the solid-electrolyte interphase (SEI), little attention has been paid to understanding its role in the mechanical failures of electrodes. Here we unveil the impact of SEI inhomogeneities on early-stage defect formation in Si electrodes. Buried under the SEI, these early-stage defects are inaccessible by most surface-probing techniques. With operando full field diffraction X-ray microscopy, we observe the formation of these defects in real time and connect their origin to a heterogeneous degree of lithiation. This heterogeneous lithiation is further correlated to inhomogeneities in topography and lithium-ion mobility in both the inner- and outer-SEI, thanks to a combination of operando atomic force microscopy, electrochemical strain microscopy and sputter-etched X-ray photoelectron spectroscopy. Our multi-modal study bridges observations across the multi-level interfaces (Si/Li x Si/inner-SEI/outer-SEI), thus offering novel insights into the impact of SEI homogeneities on the structural stability of Si-based lithium-ion batteries. Severe structural deformation during (de)lithiation is the main factor limiting the stability of Si anodes in Li-ion batteries. Here, a multi-modal approach is used to visualize these deformations in their early-stage and link them to inhomogeneities in the dual-layer solid-electrolyte interphase.

Compound refractive lenses (CRLs) are established X‐ray focusing optics, and are used to focus the beam or image the sample in many beamlines at X‐ray facilities. While CRLs are quite established, the stack of single lens elements affords a very small numerical aperture because of the thick lens profile, making them far more difficult to align than classical optical lenses that obey the thin‐lens approximation. This means that the alignment must be very precise and is highly sensitive to changes to the incident beam, often requiring regular readjustments. Some groups circumvent the full realignment procedure by using engineering controls (e.g. mounting optics) that sacrifice some of the beam's focusing precision, i.e. spot size, or resolution. While these choices minimize setup time, there are clear disadvantages. This work presents a new automated approach to align CRLs using a simple alignment apparatus that is easy to adapt and install at different types of X‐ray experiments or facilities. This approach builds on recent CRL modeling efforts, using an approach based on the Stochastic Nelder–Mead (SNM) simplex method. This method is outlined and its efficacy is demonstrated with numerical simulation that is tested in real experiments conducted at the Advanced Photon Source to confirm its performance with a synchrotron beam. This work provides an opportunity to automate key instrumentation at X‐ray facilities. The efficacy of an automatic technique to align compound refractive lenses at beamline facilities is demonstrated. The algorithm is presented in its entirety, along with the results of numerical simulations and an implementation at the Advanced Photon Source at Argonne National Laboratory, USA.

Electromechanical properties such as d 33 and strain are significantly enhanced at morphotropic phase boundaries (MPBs) between two or more different crystal structures. Many actuators, sensors and MEMS devices are therefore systems with MPBs, usually between polar phases in lead (Pb)-based ferroelectric ceramics. In the search for Pb-free alternatives, systems with MPBs between polar and non-polar phases have recently been theorized as having great promise. While such an MPB was identified in rare-earth (RE) modified bismuth ferrite (BFO) thin films, synthesis challenges have prevented its realization in ceramics. Overcoming these, we demonstrate a comparable electromechanical response to Pb-based materials at the polar-to-non-polar MPB in Sm modified BFO. This arises from ‘dual’ strain mechanisms: ferroelectric/ferroelastic switching and a previously unreported electric-field induced transition of an anti-polar intermediate phase. We show that intermediate phases play an important role in the macroscopic strain response and may have potential to enhance electromechanical properties at polar-to-non-polar MPBs.

The structures, strain fields, and defect distributions in solid materials underlie the mechanical and physical properties across numerous applications. Many modern microstructural microscopy tools characterize crystal grains, domains and defects required to map lattice distortions or deformation, but are limited to studies of the (near) surface. Generally speaking, such tools cannot probe the structural dynamics in a way that is representative of bulk behavior. Synchrotron X-ray diffraction based imaging has long mapped the deeply embedded structural elements, and with enhanced resolution, dark field X-ray microscopy (DFXM) can now map those features with the requisite nm-resolution. However, these techniques still suffer from the required integration times due to limitations from the source and optics. This work extends DFXM to X-ray free electron lasers, showing how the 10 12 photons per pulse available at these sources offer structural characterization down to 100 fs resolution (orders of magnitude faster than current synchrotron images). We introduce the XFEL DFXM setup with simultaneous bright field microscopy to probe density changes within the same volume. This work presents a comprehensive guide to the multi-modal ultrafast high-resolution X-ray microscope that we constructed and tested at two XFELs, and shows initial data demonstrating two timing strategies to study associated reversible or irreversible lattice dynamics.

This paper outlines measurement and analysis methodologies created for determining the structural responses of electroceramics to an electric field. A sample stage is developed to apply electric fields to ceramic materials at elevated temperatures during neutron diffraction experiments. The tested voltages and temperatures range from −20 kV to +20 kV and room temperature to 200 °C, respectively. The use of the sample environment for measuring the response of ferroelectric ceramics to an electrical stimulus is demonstrated on the instrument Wombat, a monochromatic neutron diffractometer employing a curved positive sensitive detector. Methodologies are proposed to account for the geometrical effects when vector fields are applied to textured materials with angularly dispersive detector geometries. Representative results are presented for the ferroelectric (Bi 1/2 Na 1/2 )TiO 3 -6%BaTiO 3 (BNT-6BT) which show both phase transformation and ferroelectric domain texturing under the application of an electric field. This experimental and analysis approach is well suited for time-resolved measurements such as stroboscopic and in situ studies on a variety of electro-active materials.

The characteristic functionality of ferroelectric materials is due to the symmetry of their crystalline structure. As such, ferroelectrics lend themselves to design approaches that manipulate this structural symmetry by introducing extrinsic strain. Using in situ dark-field X-ray microscopy to map lattice distortions around deeply embedded domain walls and grain boundaries in BaTiO3, we reveal that symmetry-breaking strain fields extend up to several micrometres from domain walls. As this exceeds the average domain width, no part of the material is elastically relaxed, and symmetry is universally broken. Such extrinsic strains are pivotal in defining the local properties and self-organization of embedded domain walls, and must be accounted for by emerging computational approaches to material design.

Dark-field x-ray microscopy is a new way to three-dimensionally map lattice strain and orientation in crystalline matter. It is analogous to dark-field electron microscopy in that an objective lens magnifies diffracting features of the sample; however, the use of high-energy synchrotron x-rays means that these features can be large, deeply embedded, and fully mapped in seconds to minutes. Simple reconfiguration of the x-ray objective lens allows intuitive zooming between different scales down to a spatial and angular resolution of 100 nm and 0.001°, respectively. Three applications of the technique are presented—mapping the evolution of subgrains during the processing of plastically deformed aluminum, mapping domains and strain fields in ferroelectric crystals, and the three-dimensional mapping of strain fields around individual dislocations. This ability to directly characterize complex, multiscale phenomena in situ is a key step toward formulating and validating multiscale models that account for the entire heterogeneity of materials.

Dark-field x-ray microscopy is intended for the acquisition of three -dimensional (3D) movies of the nanostructure (grains, domains, and dislocations) and the associated local strain within bulk materials. It is analogous to dark-field electron microscopy in that an objective lens magnifies diffracting features of the sample. The use of high-energy synchrotron x-rays, however, means that these microstructural features can be large and deeply embedded. The spatial and angular resolution is on the order of 100 nm and 0.001°, respectively, and full maps can be recorded in seconds to minutes. Four applications of the technique are presented—domain switching in ferroelectrics, processing of metals, microstructural characterization of biominerals, and visualization of dislocations. The ability to directly characterize complex, multiscale phenomena in situ —and in 3D—is a key step toward formulating and validating multiscale models that account for the entire heterogeneity of materials.