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At the nanoscale, elastic strain and crystal defects largely influence the properties and functionalities of materials. The ability to predict the structural evolution of catalytic nanocrystals during the reaction is of primary importance for catalyst design. However, to date, imaging and characterising the structure of defects inside a nanocrystal in three-dimensions and in situ during reaction has remained a challenge. We report here an unusual twin boundary migration process in a single platinum nanoparticle during CO oxidation using Bragg coherent diffraction imaging as the characterisation tool. Density functional theory calculations show that twin migration can be correlated with the relative change in the interfacial energies of the free surfaces exposed to CO. The x-ray technique also reveals particle reshaping during the reaction. In situ and non-invasive structural characterisation of defects during reaction opens new avenues for understanding defect behaviour in confined crystals and paves the way for strain and defect engineering. At the nanoscale, elastic strain and crystal defects largely influence the properties and functionalities of materials. Here, the authors report an unusual twin boundary migration process in a single platinum nanoparticle during carbon monoxide oxidation using Bragg coherent diffraction imaging.

We explore the use of continuous scanning during data acquisition for Bragg coherent diffraction imaging, i.e., where the sample is in continuous motion. The fidelity of continuous scanning Bragg coherent diffraction imaging is demonstrated on a single Pt nanoparticle in a flow reactor at 400 ∘ C in an Ar-based gas flowed at 50 ml/min. We show a reduction of 30% in total scan time compared to conventional step-by-step scanning. The reconstructed Bragg electron density, phase, displacement and strain fields are in excellent agreement with the results obtained from conventional step-by-step scanning. Continuous scanning will allow to minimise sample instability under the beam and will become increasingly important at diffraction-limited storage ring light sources.

Nanostructures with specific crystallographic planes display distinctive physico-chemical properties because of their unique atomic arrangements, resulting in widespread applications in catalysis, energy conversion or sensing. Understanding strain dynamics and their relationship with crystallographic facets have been largely unexplored. Here, we reveal in situ, in three-dimensions and at the nanoscale, the volume, surface and interface strain evolution of single supported platinum nanocrystals during reaction using coherent x-ray diffractive imaging. Interestingly, identical { hkl } facets show equivalent catalytic response during non-stoichiometric cycles. Periodic strain variations are rationalised in terms of O 2 adsorption or desorption during O 2 exposure or CO oxidation under reducing conditions, respectively. During stoichiometric CO oxidation, the strain evolution is, however, no longer facet dependent. Large strain variations are observed in localised areas, in particular in the vicinity of the substrate/particle interface, suggesting a significant influence of the substrate on the reactivity. These findings will improve the understanding of dynamic properties in catalysis and related fields. Understanding strain dynamics and their relationship with crystallographic facets have been largely unexplored. Here the authors demonstrate how the 3D lattice displacement and strain evolution depend on the crystallographic facets of Pt nanoparticles during CO oxidation reaction, providing new insights in the relationship between facet-related surface strain and chemistry.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Bragg coherent X-ray diffraction imaging (BCDI) has emerged as a powerful technique to image the local displacement field and strain in nanocrystals, in three dimensions with nanometric spatial resolution. However, BCDI relies on both dataset collection and phase retrieval algorithms that can induce artefacts in the reconstruction. Phase retrieval algorithms are based on the fast Fourier transform (FFT). We demonstrate how to calculate the displacement field inside a nanocrystal from its reconstructed phase depending on the mathematical convention used for the FFT. We use numerical simulations to quantify the influence of experimentally unavoidable detector deficiencies such as blind areas or limited dynamic range as well as post-processing filtering on the reconstruction. We also propose a criterion for the isosurface determination of the object, based on the histogram of the reconstructed modulus. Finally, we study the capability of the phasing algorithm to quantitatively retrieve the surface strain ( i.e ., the strain of the surface voxels). This work emphasizes many aspects that have been neglected so far in BCDI, which need to be understood for a quantitative analysis of displacement and strain based on this technique. It concludes with the optimization of experimental parameters to improve throughput and to establish BCDI as a reliable 3D nano-imaging technique.

The quantification and localization of elastic strains and defects in crystals are necessary to control and predict the functioning of materials. The X-ray imaging of strains has made very impressive progress in recent years. On the one hand, progress in optical elements for focusing X-rays now makes it possible to carry out X-ray diffraction mapping with a resolution in the 50–100 nm range, while lensless imaging techniques reach a typical resolution of 5–10 nm. This continuous evolution is also a consequence of the development of new two-dimensional detectors with hybrid pixels whose dynamics, reading speed and low noise level have revolutionized measurement strategies. In addition, a new accelerator ring concept (HMBA network: hybrid multi-bend achromat lattice) is allowing a very significant increase (a factor of 100) in the brilliance and coherent flux of synchrotron radiation facilities, thanks to the reduction in the horizontal size of the source. This review is intended as a progress report in a rapidly evolving field. The next ten years should allow the emergence of three-dimensional imaging methods of strains that are fast enough to follow, in situ, the evolution of a material under stress or during a transition. Handling massive amounts of data will not be the least of the challenges.

The microstructure of a sub-micrometric gold crystal during nanoindentation is visualized by in situ multi-wavelength Bragg coherent X-ray diffraction imaging. The gold crystal is indented using a custom-built atomic force microscope. A band of deformation attributed to a shear band oriented along the (221) lattice plane is nucleated at the lower left corner of the crystal and propagates towards the crystal center with increasing applied mechanical load. After complete unloading, an almost strain-free and defect-free crystal is left behind, demonstrating a pseudo-elastic behavior that can only be studied by in situ imaging while it is invisible to ex situ examinations. The recovery is probably associated with reversible dislocations nucleation/annihilation at the side surface of the particle and at the particle-substrate interface, a behavior that has been predicted by atomistic simulations. The full recovery of the particle upon unloading sheds new light on extraordinary mechanical properties of metal nanoparticles obtained by solid-state dewetting.

The simultaneous measurement of two Bragg reflections by Bragg coherent X-ray diffraction is demonstrated on a twinned Au crystal, which was prepared by the solid-state dewetting of a 30 nm thin gold film on a sapphire substrate. The crystal was oriented on a goniometer so that two lattice planes fulfill the Bragg condition at the same time. The Au 111 and Au 200 Bragg peaks were measured simultaneously by scanning the energy of the incident X-ray beam and recording the diffraction patterns with two two-dimensional detectors. While the former Bragg reflection is not sensitive to the twin boundary, which is oriented parallel to the crystal–substrate interface, the latter reflection is only sensitive to one part of the crystal. The volume ratio between the two parts of the twinned crystal is about 1:9, which is also confirmed by Laue microdiffraction of the same crystal. The parallel measurement of multiple Bragg reflections is essential for future in situ and operando studies, which are so far limited to either a single Bragg reflection or several in series, to facilitate the precise monitoring of both the strain field and defects during the application of external stimuli.

For the characterization of the mechanical properties of materials the precise measurements of stress‐strain curves is indispensable. In situ nano‐mechanical testing setups, however, may lack the precision either in terms of strain or stress determination. Recently, the custom‐built scanning force microscope SFINX was developed which is compatible with third‐generation synchrotron end‐stations allowing for in situ nano‐mechanical tests in combination with nanofocused synchrotron x‐ray diffraction that is highly sensitive to strain and defects. The usage of a self‐actuating and self‐sensing cantilever tremendously increases the compactness of the system but lacks deflection sensitivity and, thus the force measurement. This deficiency is resolved by in situ monitoring the diffraction peaks of the Si cantilever by Laue microdiffraction during the nano‐indentation of a gold crystal. The orientation and, hence, the deflection of the Si cantilever is deduced from the displacement of the Si Laue spots on the detector giving force accuracies of better than 90 nN. At the same time, the dislocation density in the indented Au crystal is tracked by monitoring the Au Laue spots eventually resulting in complete stress‐dislocation density curves. The precise measurement of both stress and strain is indispensable for the accurate characterization of mechanical properties, which is however difficult in crowded environments. Here, the force measurement with a resolution of 90 nN is realized by in situ monitoring the AFM cantilever deflection by Laue microdiffraction during nano‐indentation and simultaneously measuring the dislocation density in the indented gold crystal.

The orientation relationships (ORs) of copper crystals on a sapphire substrate equilibrated at 1253 K are presented. They barely depend on the procedures used in sample preparation, i.e. dewetting of a copper film in the liquid state or in the solid state. The most frequent OR found is Cu(111) || Al 2 O 3 and Cu within few degrees from Al 2 O 3 [0001]. A secondary, lower frequency OR is also observed: Cu(001) || Al 2 O 3 with Cu within a few degrees from either Al 2 O 3 or Al 2 O 3 [0001]. These ORs do not follow the Fecht and Gleiter model which proposes that dense directions of the metal should align with dense directions of the oxide. On annealing, even at a temperature about half of the melting point of sapphire, fast diffusion of sapphire at the copper/sapphire interface is observed: the copper particles tend to achieve their interfacial equilibrium shapes by sinking into the substrate, and sapphire ridges form at the triple line. Finally, it is shown that the Cu(111) || Al 2 O 3 interface remains flat at the atomic scale, and is therefore part of the copper/sapphire equilibrium interfacial shape.