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As a critical component of coherent X-ray diffraction imaging (CDI), phase retrieval has been extensively applied in X-ray structural science to recover the 3D morphological information inside measured particles. Despite meeting all the oversampling requirements of Sayre and Shannon, current phase retrieval approaches still have trouble achieving a unique inversion of experimental data in the presence of noise. Here, we propose to overcome this limitation by incorporating a 3D Machine Learning (ML) model combining (optional) supervised learning with transfer learning. The trained ML model can rapidly provide an immediate result with high accuracy which could benefit real-time experiments, and the predicted result can be further refined with transfer learning. More significantly, the proposed ML model can be used without any prior training to learn the missing phases of an image based on minimization of an appropriate ‘loss function’ alone. We demonstrate significantly improved performance with experimental Bragg CDI data over traditional iterative phase retrieval algorithms.

Palladium absorbs large volumetric quantities of hydrogen at room temperature and ambient pressure, making the palladium hydride system a promising candidate for hydrogen storage. Here, we use Bragg coherent diffraction imaging to map the strain associated with defects in three dimensions before and during the hydride phase transformation of an individual octahedral palladium nanoparticle, synthesized using a seed-mediated approach. The displacement distribution imaging unveils the location of the seed nanoparticle in the final nanocrystal. By comparing our experimental results with a finite-element model, we verify that the seed nanoparticle causes a characteristic displacement distribution of the larger nanocrystal. During the hydrogen exposure, the hydride phase is predominantly formed on one tip of the octahedra, where there is a high number of lower coordinated Pd atoms. Our experimental and theoretical results provide an unambiguous method for future structure optimization of seed-mediated nanoparticle growth and in the design of palladium-based hydrogen storage systems. Palladium can absorb high volumes of hydrogen, but the morphology and 3D displacements occurring during palladium hydride phase formation are not fully characterized in the literature. Here, the authors use Bragg coherent diffraction imaging to map the strain within an individual palladium nanoparticle before and during hydride phase transformation, identifying a characteristic displacement caused by the seed particle in the nanocrystal.

All-solid-state lithium batteries promise significant improvements in energy density and safety over traditional liquid electrolyte batteries. The Al-doped Li7La3Zr2O12 (LLZO) solid-state electrolyte shows excellent potential given its high ionic conductivity and good thermal, chemical, and electrochemical stability. Nevertheless, further improvements on electrochemical and mechanical properties of LLZO call for an in-depth understanding of its local microstructure. Here, we employ Bragg coherent diffractive imaging to investigate the atomic displacements inside single grains of LLZO with various Al-doping concentrations, resulting in cubic, tetragonal, and cubic-tetragonal mixed structures. We observe coexisting domains of different crystallographic orientations in the tetragonal structure. We further show that Al doping leads to crystal defects such as dislocations and phase boundaries in the mixed- and cubic-phase grain. This study addresses the effect of Al doping on the nanoscale structure within individual grains of LLZO, which is informative for the future development of solid-state batteries.

Focused ion beam (FIB) techniques are commonly used to machine, analyse and image materials at the micro- and nanoscale. However, FIB modifies the integrity of the sample by creating defects that cause lattice distortions. Methods have been developed to reduce FIB-induced strain, however these protocols need to be evaluated for their effectiveness. Here we use non-destructive Bragg coherent X-ray diffraction imaging to study the in situ annealing of FIB-milled gold microcrystals. We simultaneously measure two non-collinear reflections for two different crystals during a single annealing cycle, demonstrating the ability to reliably track the location of multiple Bragg peaks during thermal annealing. The thermal lattice expansion of each crystal is used to calculate the local temperature. This is compared to thermocouple readings, which are shown to be substantially affected by thermal resistance. To evaluate the annealing process, we analyse each reflection by considering facet area evolution, cross-correlation maps of displacement field and binarised morphology, and average strain plots. The crystal's strain and morphology evolve with increasing temperature, which is likely to be caused by the diffusion of gallium in gold below ~280{\deg}C and the self-diffusion of gold above ~280{\deg}C. The majority of FIB-induced strains are removed by 380-410\degree C, depending on which reflection is being considered. Our observations highlight the importance of measuring multiple reflections to unambiguously interpret material behaviour., Comment: 51 pages, 16 figures

Fundamental understanding of structural changes during catalytic reactions is crucial to understanding the underlying mechanisms and optimizing efficiencies. Surface energy and related catalytic mechanisms are widely studied. However, the catalyst lattice deformation induced by catalytic processes is not well understood. Here, we study the strain in an individual platinum (Pt) nanoparticle (NP) using Bragg coherent diffraction imaging under in situ oxidation and reduction reactions. When Pt NPs are exposed to H

Understanding catalysts strain dynamic behaviours is crucial for the development of cost-effective, efficient, stable and long-lasting catalysts. Here, we reveal in situ three-dimensional strain evolution of single gold nanocrystals during a catalytic CO oxidation reaction under operando conditions with coherent X-ray diffractive imaging. We report direct observation of anisotropic strain dynamics at the nanoscale, where identically crystallographically-oriented facets are qualitatively differently affected by strain leading to preferential active sites formation. Interestingly, the single nanoparticle elastic energy landscape, which we map with attojoule precision, depends on heating versus cooling cycles. The hysteresis observed at the single particle level is following the normal/inverse hysteresis loops of the catalytic performances. This approach opens a powerful avenue for studying, at the single particle level, catalytic nanomaterials and deactivation processes under operando conditions that will enable profound insights into nanoscale catalytic mechanisms., Direct visualisation of site-specific strain variations of catalysts is needed to better understand catalytic properties. Here, the authors determine with attojoule precision that the well-known catalytic hysteresis phenomenon occurs at single particle level and involves three-dimensional strain field.

Oxidation of magnetite (Fe3O4) has broad implications in geochemistry, environmental science and materials science. Spatially resolving strain fields and defect evolution during oxidation of magnetite provides further insight into its reaction mechanisms. Here we show that the morphology and internal strain distributions within individual nano-sized (~400 nm) magnetite crystals can be visualized using Bragg coherent diffractive imaging (BCDI). Oxidative dissolution in acidic solutions leads to increases in the magnitude and heterogeneity of internal strains. This heterogeneous strain likely results from lattice distortion caused by Fe(II) diffusion that leads to the observed domains of increasing compressive and tensile strains. In contrast, strain evolution is less pronounced during magnetite oxidation at elevated temperature in air. These results demonstrate that oxidative dissolution of magnetite can induce a rich array of strain and defect structures, which could be an important factor that contributes to the high reactivity observed on magnetite particles in aqueous environment., Oxidation of magnetite has broad implications in geochemistry and environmental science, but its reaction mechanisms are not fully understood yet. Here the authors use Bragg coherent diffractive imaging to show oxidative dissolution of magnetite inducing a rich array of strain and defect structures.

Using operando Bragg coherent x-ray diffraction imaging, we visualised three-dimensionally a single twinned-gold nanocrystal during the CO oxidation reaction. We describe the defect dynamics process occurring under operating conditions and indicate the correlation between the nucleation of highly strained regions at the surface of the nanocrystal and its catalytic activity. Understanding the twinning deformation mechanism sheds light on the creation of active sites, and could well contribute to the understanding of the catalytic behaviour of other catalysts. With the start-up of 4th generation synchrotron sources, we anticipate that coherent hard x-ray diffraction imaging techniques will play a major role in imaging in situ chemical processes.

In this work, ferroelastic domain walls inside ${\mathrm{BaTiO}}_{3}$ (BTO) tetragonal nanocrystals are distinguished by Bragg peak position and studied with Bragg coherent x-ray diffraction imaging (BCDI). Convergence-related features of the BCDI method for strongly phased objects are reported. A ferroelastic domain wall inside a BTO crystal has been tracked and imaged across the tetragonal-cubic phase transition and proves to be reversible. The linear relationship of relative displacement between two twin domains with temperature is measured and shows a different slope for heating and cooling, while the tetragonality reproduces well over temperature changes in both directions. An edge dislocation is also observed and found to annihilate when heating the crystal close to the phase transition temperature.

X-ray Bragg coherent diffraction imaging (BCDI) has been demonstrated as a powerful 3D microscopy approach for the investigation of sub-micrometre-scale crystalline particles. The approach is based on the measurement of a series of coherent Bragg diffraction intensity patterns that are numerically inverted to retrieve an image of the spatial distribution of the relative phase and amplitude of the Bragg structure factor of the diffracting sample. This 3D information, which is collected through an angular rotation of the sample, is necessarily obtained in a non-orthogonal frame in Fourier space that must be eventually reconciled. To deal with this, the approach currently favored by practitioners (detailed in Part I) is to perform the entire inversion in conjugate non-orthogonal real- and Fourier-space frames, and to transform the 3D sample image into an orthogonal frame as a post-processing step for result analysis. In this article, which is a direct follow-up of Part I, two different transformation strategies are demonstrated, which enable the entire inversion procedure of the measured data set to be performed in an orthogonal frame. The new approaches described here build mathematical and numerical frameworks that apply to the cases of evenly and non-evenly sampled data along the direction of sample rotation (i.e. the rocking curve). The value of these methods is that they rely on the experimental geometry, and they incorporate significantly more information about that geometry into the design of the phase-retrieval Fourier transformation than the strategy presented in Part I. Two important outcomes are (1) that the resulting sample image is correctly interpreted in a shear-free frame and (2) physically realistic constraints of BCDI phase retrieval that are difficult to implement with current methods are easily incorporated. Computing scripts are also given to aid readers in the implementation of the proposed formalisms.

The commissioning of a movable X-ray monochromator at the 34-ID-C endstation of the Advanced Photon Source is reported. The new instrument allows indexing of nanocrystals with Laue diffraction and collecting multi-reflection BCDI data., Measurement modalities in Bragg coherent diffraction imaging (BCDI) rely on finding a signal from a single nanoscale crystal object which satisfies the Bragg condition among a large number of arbitrarily oriented nanocrystals. However, even when the signal from a single Bragg reflection with (hkl) Miller indices is found, the crystallographic axes on the retrieved three-dimensional (3D) image of the crystal remain unknown, and thus localizing in reciprocal space other Bragg reflections becomes time-consuming or requires good knowledge of the orientation of the crystal. Here, the commissioning of a movable double-bounce Si (111) monochromator at the 34-ID-C endstation of the Advanced Photon Source is reported, which aims at delivering multi-reflection BCDI as a standard tool in a single beamline instrument. The new instrument enables, through rapid switching from monochromatic to broadband (pink) beam, the use of Laue diffraction to determine crystal orientation. With a proper orientation matrix determined for the lattice, one can measure coherent diffraction patterns near multiple Bragg peaks, thus providing sufficient information to image the full strain tensor in 3D. The design, concept of operation, the developed procedures for indexing Laue patterns, and automated measuring of Bragg coherent diffraction data from multiple reflections of the same nanocrystal are discussed.

Structural symmetry breaking and recovery in condensed-matter systems are closely related to exotic physical properties such as superconductivity (SC), magnetism, spin density waves, and charge density waves (CDWs). The interplay between different order parameters is intricate and often subject to intense debate, as in the case of CDW order and superconductivity. In ${\mathrm{La}}_{1.875}{\mathrm{Ba}}_{0.125}{\mathrm{CuO}}_{4}$ (LBCO), the low-temperature structural domain walls are hypothesized as nanometer-scale pinning sites for the CDWs. Coherent x-ray diffraction techniques have been employed here to visualize the domain structures associated with these symmetry changes directly during phase transition. We have pushed Bragg coherent diffractive imaging (BCDI) into the cryogenic regime where most phase transitions in quantum materials reside. Utilizing BCDI, we image the structural evolution of LBCO microcrystal samples during the high-temperature tetragonal to low-temperature orthorhombic (LTO) phase transition. Our results show the formation of LTO domains close to the transition temperature and how the domain size decreases with temperature. The number of domains follows the secondary order parameter (or orthorhombic strain) measurement with a critical exponent that is consistent with the three-dimensional universality class.

Emerging two-dimensional (2-D) materials such as transition-metal dichalcogenides show great promise as viable alternatives for semiconductor and optoelectronic devices that progress beyond silicon. Performance variability, reliability, and stochasticity in the measured transport properties represent some of the major challenges in such devices. Native strain arising from interfacial effects due to the presence of a substrate is believed to be a major contributing factor. A full three-dimensional (3-D) mapping of such native nanoscopic strain over micron length scales is highly desirable for gaining a fundamental understanding of interfacial effects but has largely remained elusive. Here, we employ coherent X-ray diffraction imaging to directly image and visualize in 3-D the native strain along the (002) direction in a typical multilayered (∼100–350 layers) 2-D dichalcogenide material (WSe2) on silicon substrate. We observe significant localized strains of ∼0.2% along the out-of-plane direction. Experimen...

Watching defects in heated thin films The response of materials to external conditions depends on small-scale features such as defects and grain boundaries. Yau et al. heated gold thin films and used coherent x-ray diffractive imaging to track how these microstructures developed during grain growth (see the Perspective by Suter). The technique allowed nondestructive visualization of the features in three dimensions. The method should help link external stimuli to material response through changes in microstructure, thereby allowing development of novel materials through microstructural engineering. Science , this issue p. 739 ; see also p. 704

Dissolution is critical to nanomaterial stability, especially for partially dealloyed nanoparticle catalysts. Unfortunately, highly active catalysts are often not stable in their reactive environments, preventing widespread application. Thus, focusing on the structure–stability relationship at the nanoscale is crucial and will likely play an important role in meeting grand challenges. Recent advances in imaging capability have come from electron, X-ray, and other techniques but tend to be limited to specific sample environments and/or two-dimensional images. Here, we report investigations into the defect-stability relationship of silver nanoparticles to voltage-induced electrochemical dissolution imaged in situ in three-dimensional detail by Bragg coherent diffractive imaging. We first determine the average dissolution kinetics by stationary probe rotating disk electrode in combination with inductively coupled plasma mass spectrometry, which allows in situ measurement of Ag+ ion formation. We then observe...

Defects can affect all aspects of a material by altering its electronic properties and controlling its chemical reactivity. At defect sites, preferential adsorption of reactants and/or formation of chemical species at active sites are observed in heterogeneous catalysis. Understanding the structural response at defect sites during catalytic reactions provides a unique opportunity to exploit defect control of nanoparticle-based catalysts. However, it remains difficult to characterize the strain and defect evolution for a single nanocrystal catalyst in situ. Here, we report Bragg coherent X-ray diffraction imaging of defect dynamics in an individual Pt nanoparticle during catalytic methane oxidation. We observed that the initially tensile strained regions of the crystal became seed points for the development of further strain and subsequent disappearance of diffraction density during oxidation reactions. Our detailed understanding of the catalytically induced deformation at the defect sites and observed reversibility during the relevant steps of the catalytic oxidation process provide important insights of defect control and engineering of heterogeneous catalysts.

Bragg coherent diffraction imaging (BCDI), a well-established technique for imaging the internal strain of nanoparticles, was used to image the internal compositional distribution of binary alloys in thermal equilibrium. The images experimentally obtained for Pd-Rh alloy nanoparticles are presented and discussed. A direct correspondence between the lattice strain and the compositional deviation is discussed with the derivation of the BCDI displacement field aided by illustrations. The correspondence suggests that the longitudinal derivative of the displacement field, the strain induced by compositional heterogeneity, can be quantitatively converted to 3D images of the compositional deviation from the particle average by using Vegard’s law. It also suggests that the transverse derivative can be qualitatively associated with the disorder of Bragg planes. The studied Pd-Rh alloy nanoparticle exhibited internal composition heterogeneity; the Rh composition tends to be high at edges and corners between facets and gradually decreases from the surface to the core of the particle.

Imaging the dynamical response of materials following ultrafast excitation can reveal energy transduction mechanisms and their dissipation pathways, as well as material stability under conditions far from equilibrium. Such dynamical behavior is challenging to characterize, especially operando at nanoscopic spatiotemporal scales. In this letter, we use X-ray coherent diffractive imaging to show that ultrafast laser excitation of a ZnO nanocrystal induces a rich set of deformation dynamics including characteristic "hard" or inhomogeneous and "soft" or homogeneous modes at different time scales, corresponding respectively to the propagation of acoustic phonons and resonant oscillation of the crystal. By integrating the 3D nanocrystal structure obtained from the ultrafast X-ray measurements with a continuum thermo-electro-mechanical finite element model, we elucidate the deformation mechanisms following laser excitation, in particular, a torsional mode that generates a 50% greater electric potential gradient than that resulting from the flexural mode. Understanding of the time-dependence of these mechanisms on ultrafast scales has significant implications for development of new materials for nanoscale power generation.

We synthesized a planar pDPPTTi-OD polymer based on diketopyrrolopyrrole (DPP) and thieno [2,3- b ]thiophene (TTi) and investigated the electrical properties of the pDPPTTi-OD polymer. pDPPTTi-OD films displayed a low optical bandgap of 1.57 eV, and HOMO and LUMO levels of −5.40 and −3.74 eV, respectively. The 150°C-annealed pDPPTTi-OD films showed a high hole mobility of 0.16 cm 2 V −1 s −1 in organic thin-film transistor (OTFT) devices. The photovoltaic properties of polymer solar cells (PSCs) incorporating the pDPPTTi-OD were also measured. A pDPPTTi-OD:PC 71 BM blend film was spin-coated at 25, 70 and 90 °C. High-temperature processing significantly improved the power conversion efficiency of PSCs by effectively reducing the PC 71 BM domain sizes, which improved the miscibility between pDPPTTi-OD and PC 71 BM. This work demonstrated that the TTi moiety is a useful donor building block for high- performance D–A type polymers in OTFTs and PSCs, and that processing temperatures should be controlled to fully realize the materials' beneficial intrinsic properties.

A method is presented to simplify Bragg coherent X-ray diffraction imaging studies of complex heterogeneous crystalline materials with a two-stage screening/imaging process that utilizes polychromatic and monochromatic coherent X-rays and is compatible within situsample environments. Coherent white-beam diffraction is used to identify an individual crystal particle or grain that displays desired properties within a larger population. A three-dimensional reciprocal-space map suitable for diffraction imaging is then measured for the Bragg peak of interest using a monochromatic beam energy scan that requires no sample motion, thus simplifyingin situchamber design. This approach was demonstrated with Au nanoparticles and will enable, for example, individual grains in a polycrystalline material of specific orientation to be selected, then imaged in three dimensions while under load.

Physical review letters 123(24), 246001 (2019). doi:10.1103/PhysRevLett.123.246001, Bimetallic catalysts can undergo segregation or redistribution of the metals driven by oxidizing andreducing environments. Bragg coherent diffraction imaging (BCDI) was used to relate displacement fieldsto compositional distributions in crystalline Pt-Rh alloy nanoparticles. Three-dimensional images ofinternal composition showed that the radial distribution of compositions reverses partially between thesurface shell and the core when gas flow changes between O2 and H2. Our observation suggests that theelemental segregation of nanoparticle catalysts should be highly active during heterogeneous catalysis andcan be a controlling factor in synthesis of electrocatalysts. In addition, our study exemplifies applications ofBCDI for in situ 3D imaging of internal equilibrium compositions in other bimetallic alloy nanoparticles., Published by APS, College Park, Md.

The crystalline strain properties of nanoparticles have broad implications in a number of emerging fields, including quantum and biological sensing in which heterogeneous internal strain fields are detrimental to performance. Here we used synchrotron-based Bragg coherent x-ray diffraction imaging (BCDI) to measure three-dimensional lattice strain fields within individual 3C-SiC nanoparticles, a candidate host material for quantum sensing, as a function of temperature during and after annealing up to ${900}^{\phantom{\rule{0.16em}{0ex}}\ensuremath{\circ}}\mathrm{C}$. We observed pronounced homogenization of the initial strain field at temperatures above ${500}^{\phantom{\rule{0.16em}{0ex}}\ensuremath{\circ}}\mathrm{C}$, and we find that the surface layers and central volumes of the nanoparticles reduce strain at similar rates, suggesting a uniform healing mechanism. Thus, we attribute the observed strain homogenization to activation of mobile point defects that annihilate and improve the overall quality of the crystal lattice. This work also establishes the feasibility of performing BCDI at high temperatures (up to ${900}^{\phantom{\rule{0.16em}{0ex}}\ensuremath{\circ}}\mathrm{C}$) to map structural hystereses relevant to the processing of quantum nanomaterials.

Nature Communications 9, 3422 (2018). doi:10.1038/s41467-018-05464-2, High catalytic efficiency in metal nanocatalysts is attributed to large surface area to volume ratios and an abundance of under-coordinated atoms that can decrease kinetic barriers. Although overall shape or size changes of nanocatalysts have been observed as a result of catalytic processes, structural changes at low-coordination sites such as edges, remain poorly understood. Here, we report high-lattice distortion at edges of Pt nanocrystals during heterogeneous catalytic methane oxidation based on in situ 3D Bragg coherent X-ray diffraction imaging. We directly observe contraction at edges owing to adsorption of oxygen. This strain increases during methane oxidation and it returns to the original state after completing the reaction process. The results are in good agreement with finite element models that incorporate forces, as determined by reactive molecular dynamics simulations. Reaction mechanisms obtained from in situ strain imaging thus provide important insights for improving catalysts and designing future nanostructured catalytic materials., Published by Nature Publishing Group, London

We demonstrate that the resolution of three-dimensional (3D) real-space images obtained from Bragg x-ray coherent diffraction measurements is direction dependent. We propose and demonstrate the effectiveness of a metric to determine the spatial resolution of images that accounts for the direc- tional dependence. The measured direction dependent resolution of ~ 4-9nm is about 2 times higher than the best previously obtained 3D measurements. Finally, we quantify the relationship between the resolution of recovered real-space images and dosage, and discuss its implications in the light of next generation synchrotrons.

Visualizing the dynamical response of material heterointerfaces is increasingly important for the design of hybrid materials and structures with tailored properties for use in functional devices. In situ characterization of nanoscale heterointerfaces such as metal-semiconductor interfaces, which exhibit a complex interplay between lattice strain, electric potential, and heat transport at subnanosecond time scales, is particularly challenging. In this work, we use a laser pump/X-ray probe form of Bragg coherent diffraction imaging (BCDI) to visualize in three-dimension the deformation of the core of a model core/shell semiconductor-metal (ZnO/Ni) nanorod following laser heating of the shell. We observe a rich interplay of radial, axial, and shear deformation modes acting at different time scales that are induced by the strain from the Ni shell. We construct experimentally informed models by directly importing the reconstructed crystal from the ultrafast experiment into a thermo-electromechanical continuum model. The model elucidates the origin of the deformation modes observed experimentally. Our integrated imaging approach represents an invaluable tool to probe strain dynamics across mixed interfaces under operando conditions.

Mesoscale thermal transport is of fundamental interest and practical importance in materials such as thermoelectrics. Coherent lattice vibrations (acoustic phonons) govern thermal transport in crystalline solids and are affected by the shape, size, and defect density in nanoscale materials. The advent of hard x-ray free electron lasers (XFELs) capable of producing ultrafast x-ray pulses has significantly impacted the understanding of acoustic phonons by enabling their direct study with x-rays. However, previous studies have reported ensemble-averaged results that cannot distinguish the impact of mesoscale heterogeneity on the phonon dynamics. Here we use Bragg coherent diffractive imaging (BCDI) to resolve the 4D evolution of the acoustic phonons in a single zinc oxide rod with a spatial resolution of 50 nm and a temporal resolution of 25 picoseconds. We observe homogeneous (lattice breathing/rotation) and inhomogeneous (shear) acoustic phonon modes, which are compared to finite element simulations. We investigate the possibility of changing phonon dynamics by altering the crystal through acid etching. We find that the acid heterogeneously dissolves the crystal volume, which will significantly impact the phonon dynamics. In general, our results represent the first step towards understanding the effect of structural properties at the individual crystal level on phonon dynamics.

International audience; We present and demonstrate a formalism by which three dimensional (3D) Bragg x-ray coherent diffraction imaging (BCDI) can be implemented without moving the sample by scanning the energy of the incident x-ray beam. This capability is made possible by introducing a 3D Fourier transform that accounts for x-ray wavelength variability. We demonstrate the approach by inverting coherent Bragg diffraction patterns from a gold nanocrystal measured with an x-ray energy scan. Variable-wavelength BCDI will expand the breadth of feasible in situ 3D strain imaging experiments towards more diverse materials environments, especially where sample manipulation is difficult.

Bragg coherent x-ray diffractive imaging is a powerful technique for investigating dynamic nanoscale processes in nanoparticles immersed in reactive, realistic environments. Its temporal resolution is limited, however, by the oversampling requirements of three-dimensional phase retrieval. Here, we show that incorporating the entire measurement time series, which is typically a continuous physical process, into phase retrieval allows the oversampling requirement at each time step to be reduced, leading to a subsequent improvement in the temporal resolution by a factor of 2-20 times. The increased time resolution will allow imaging of faster dynamics and of radiation-dose-sensitive samples. Furthermore, this approach, which we call "chrono CDI," may find use in improving the time resolution in other imaging techniques.

Dealloying is a process whereby selective dissolution results in a porous, strained structure often with new properties. The process is of both intrinsic and applied interest, and recently has been used to make highly active catalysts. The porosity has been studied using electron microscopy while the dealloying-induced strain has been studied at the ensemble level using X-ray diffraction. Despite the importance of local, for example, at the individual particle or grain level, strain in controlling the properties of the dealloyed material, it remains unresolved due to the difficulty of imaging 3D strain distributions with nanometer resolution in reactive environments. This information could play an integral role in understanding and controlling lattice strain for a variety of applications. Here, 3D strain distributions in individual nanoparticles and thin film grains in silver–gold alloys undergoing nitric acid-induced dealloying are imaged by Bragg coherent diffractive imaging. Particles exhibit dramatic changes in their local strains due to dealloying but grains do not. The average lattice in both grains and particles contracts during dealloying. In general, the results reveal significant dealloying-induced strain heterogeneity at the nanoscale in both isolated and extended samples, which may be utilized to develop advanced nanostructures for a variety of important applications.

We observed changes in morphology and internal strain state of commercial diamond nanocrystals during high-temperature annealing. Three nanodiamonds were measured with Bragg coherent x-ray diffraction imaging, yielding three-dimensional strain-sensitive images as a function of time/temperature. Up to temperatures of 800 °C, crystals with Gaussian strain distributions with a full-width-at-half-maximum of less than 8 × 10 − 4 were largely unchanged, and annealing-induced strain relaxation was observed in a nanodiamond with maximum lattice distortions above this threshold. X-ray measurements found changes in nanodiamond morphology at temperatures above 600 °C that are consistent with graphitization of the surface, a result verified with ensemble Raman measurements.