Imaging Light-Induced Migration of Dislocations in Halide Perovskites with 3D Nanoscale Strain Mapping.

In recent years, halide perovskite materials have been used to make high-performance solar cells and light-emitting devices. However, material defects still limit device performance and stability. Here, synchrotron-based Bragg coherent diffraction imaging is used to visualize nanoscale strain fields, such as those local to defects, in halide perovskite microcrystals. Significant strain heterogeneity within MAPbBr3 (MA = CH3 NH3 + ) crystals is found in spite of their high optoelectronic quality, and both 〈100〉 and 〈110〉 edge dislocations are identified through analysis of their local strain fields. By imaging these defects and strain fields in situ under continuous illumination, dramatic light-induced dislocation migration across hundreds of nanometers is uncovered. Further, by selectively studying crystals that are damaged by the X-ray beam, large dislocation densities and increased nanoscale strains are correlated with material degradation and substantially altered optoelectronic properties assessed using photoluminescence microscopy measurements. These results demonstrate the dynamic nature of extended defects and strain in halide perovskites, which will have important consequences for device performance and operational stability.

Dual energy X-ray beam ptycho-fluorescence imaging.

X-ray ptychography and X-ray fluorescence are complementary nanoscale imaging techniques, providing structural and elemental information, respectively. Both methods acquire data by scanning a localized beam across the sample. X-ray ptychography processes the transmission signal of a coherent illumination interacting with the sample, to produce images with a resolution finer than the illumination spot and step size. By enlarging both the spot and the step size, the technique can cover extended regions efficiently. X-ray fluorescence records the emitted spectra as the sample is scanned through the localized beam and its spatial resolution is limited by the spot and step size. The requisites for fast ptychography and high-resolution fluorescence appear incompatible. Here, a novel scheme that mitigates the difference in requirements is proposed. The method makes use of two probes of different sizes at the sample, generated by using two different energies for the probes and chromatic focusing optics. The different probe sizes allow to reduce the number of acquisition steps for the joint fluorescence-ptychography scan compared with a standard single beam scan, while imaging the same field of view. The new method is demonstrated experimentally using two undulator harmonics, a Fresnel zone plate and an energy discriminating photon counting detector.

X-Ray Ptychography with a Laboratory Source.

X-ray ptychography has revolutionized nanoscale phase contrast imaging at large-scale synchrotron sources in recent years. We present here the first successful demonstration of the technique in a small-scale laboratory setting. An experiment was conducted with a liquid metal-jet x-ray source and a single photon-counting detector with a high spectral resolution. The experiment used a spot size of 5 µm to produce a ptychographic phase image of a Siemens star test pattern with a submicron spatial resolution. The result and methodology presented show how high-resolution phase contrast imaging can now be performed at small-scale laboratory sources worldwide.

Structural and compositional characteristics of Fukushima release particulate material from Units 1 and 3 elucidates release mechanisms, accident chronology and future decommissioning strategy.

The structural form and elemental distribution of material originating from different Fukushima Daiichi Nuclear Power Plant reactors (Units 1 and 3) is hereby examined to elucidate their contrasting release dynamics and the current in-reactor conditions to influence future decommissioning challenges. Complimentary computed X-ray absorption tomography and X-ray fluorescence data show that the two suites of Si-based material sourced from the different reactor Units have contrasting internal structure and compositional distribution. The known event and condition chronology correlate with the observed internal and external structures of the particulates examined, which suggest that Unit 1 ejecta material sustained a greater degree of melting than that likely derived from reactor Unit 3. In particular, we attribute the near-spherical shape of Unit 1 ejecta and their internal voids to there being sufficient time for surface tension to round these objects before the hot (and so relatively low viscosity) silicate melt cooled to form glass. In contrast, a more complex internal form associated with the sub-mm particulates invoked to originate from Unit 3 suggest a lower peak temperature, over a longer duration. Using volcanic analogues, we consider the structural form of this material and how it relates to its environmental particulate stability and the bulk removal of residual materials from the damaged reactors. We conclude that the brittle and angular Unit 3 particulate are more susceptible to further fragmentation and particulate generation hazard than the round, higher-strength, more homogenous Unit 1 material.

Compositional and structural analysis of Fukushima-derived particulates using high-resolution x-ray imaging and synchrotron characterisation techniques.

Both the three-dimensional internal structure and elemental distribution of near-field radioactive fallout particulate material released during the March 2011 accident at the Fukushima Daiichi Nuclear Power Plant is analysed using combined high-resolution laboratory and synchrotron radiation x-ray techniques. Results from this study allow for the proposition of the likely formation mechanism of the particles, as well as the potential risks associated with their existence in the environment, and the likely implications for future planned reactor decommissioning. A suite of particles is analyzed from a locality 2 km from the north-western perimeter of the site - north of the primary contaminant plume in an area formerly attributed to being contaminated by fallout from reactor Unit 1. The particles are shown to exhibit significant structural similarities; being amorphous with a textured exterior, and containing inclusions of contrasting compositions, as well as an extensive internal void volume - bimodal in its size distribution. A heterogeneous distribution of the various elemental constituents is observed inside a representative particle, which also exhibited a Fukushima-derived radiocesium (134Cs, 135Cs and 137Cs) signature with negligible natural Cs. We consider the structure and composition of the particle to suggest it formed from materials associated with the reactor Unit 1 building explosion, with debris fragments embedded into the particles surface. Such a high void ratio, comparable to geological pumice, suggests such material formed during a rapid depressurisation and is potentially susceptible to fragmentation through attrition.

Spectroscopic imaging with single acquisition ptychography and a hyperspectral detector.

We present a new method of single acquisition spectroscopic imaging with high spatial resolution. The technique is based on the combination of polychromatic synchrotron radiation and ptychographic imaging with a recently developed energy discriminating detector. We demonstrate the feasibility with a Ni-Cu test sample recorded at I13-1 of the Diamond Light Source, UK. The two elements can be clearly distinguished and the Ni absorption edge is identified. The results prove the feasibility of obtaining high-resolution structural and chemical images within a single acquisition using a polychromatic X-ray beam. The capability of resolving the absorption edge applies to a wide range of research areas, such as magnetic domains imaging and element specific investigations in biological, materials, and earth sciences. The method utilises the full available radiation spectrum and is therefore well suited for broadband radiation sources.

Provenance of uranium particulate contained within Fukushima Daiichi Nuclear Power Plant Unit 1 ejecta material.

Here we report the results of multiple analytical techniques on sub-mm particulate material derived from Unit 1 of the Fukushima Daiichi Nuclear Power Plant to provide a better understanding of the events that occurred and the environmental legacy. Through combined x-ray fluorescence and absorption contrast micro-focused x-ray tomography, entrapped U particulate are observed to exist around the exterior circumference of the highly porous Si-based particle. Further synchrotron radiation analysis of a number of these entrapped particles shows them to exist as UO2-identical to reactor fuel, with confirmation of their nuclear origin shown via mass spectrometry analysis. While unlikely to represent an environmental or health hazard, such assertions would likely change should break-up of the Si-containing bulk particle occur. However, more important to the long-term decommissioning of the reactors at the FDNPP (and environmental clean-upon), is the knowledge that core integrity of reactor Unit 1 was compromised with nuclear material existing outside of the reactors primary containment.

Ptychographic X-ray computed tomography at a high-brilliance X-ray source.

Ptychographic X-ray computed tomography is a phase-contrast imaging technique capable of retrieving three-dimensional maps of the index of refraction of the imaged volumes with nanometric resolution. Despite its unmatched reach, its application remains prerogative of a limited number of laboratories at synchrotron sources. We present a detailed description of an experimental procedure and a data analysis pipeline which can be both exploited for ptychographic X-ray computed tomography experiments at any high-brilliance X-ray source. These have been validated at the I13-1 Coherence Branchline within the first experiment of its kind to be successfully carried out on a biological sample at Diamond Light Source.

Multiscale X-ray imaging using ptychography.

The success of ptychography and other imaging experiments at third-generation X-ray sources is apparent from their increasingly widespread application and the improving quality of the images they produce both for resolution and contrast and in terms of relaxation of experimental constraints. The wider availability of highly coherent X-rays stimulates the development of several complementary techniques which have seen limited mutual integration in recent years. This paper presents a framework in which some of the established imaging techniques - with particular regard for ptychography - are flexibly applied to tackle the variable requirements occurring at typical synchrotron experiments. In such a framework one can obtain low-resolution images of whole samples and smoothly zoom in on specific regions of interest as they are revealed by switching to a higher-resolution imaging mode. The techniques involved range from full-field microscopy, to reach the widest fields of view (>mm), to ptychography, to achieve the highest resolution (<100 nm), and have been implemented at the I13 Coherence Branchline at Diamond Light Source.

Separation of three-dimensional scattering effects in tilt-series Fourier ptychography.

We investigate a strategy for separating the influence of three-dimensional scattering effects in tilt-series reconstruction, a method for computationally increasing the resolution of a transmission microscope with an objective lens of small numerical aperture, as occurs in the transmission electron microscope (TEM). Recent work with visible light refers to the method as Fourier ptychography. To date, reconstruction methods presume that the object is thin enough so that the beam tilt induces only a shift of the diffraction pattern in the back focal plane. In fact, it is well known that the diffraction pattern changes as a function of beam tilt when the object is thick. In this paper, we use a simple visible light model to demonstrate a proof-of-principle of a new reconstruction algorithm that can cope with this difficulty and compare it with the aperture-scanning method. Although the experiment uses a model specimen with just two distinct layers separated along the optic axis, it should in principle be extendable to continuous objects.

Information multiplexing in ptychography.

We show for the first time that ptychography (a form of lensless diffractive imaging) can recover the spectral response of an object through simultaneous reconstruction of multiple images that represent the object's response to a particular mode present in the illumination. We solve the phase problem for each mode independently, even though the intensity arriving at every detector pixel is an incoherent superposition of several uncorrelated diffracted waves. Until recently, the addition of incoherent modes has been seen as a nuisance in diffractive imaging: here we show that not only can the difficulties they pose be removed, but that they can also be used to discover much more information about the object. If the illumination function is also mode-specific, we show that we can also solve simultaneously for a multiplicity of such illumination modes. The work opens exciting possibilities for information multiplexing in ptychography over all visible, X-ray and electron wavelengths.