The availability of ultrafast pulses of coherent hard x-rays from the Linac Coherent Light Source opens new opportunities for studies of atomic-scale dynamics in amorphous materials. Here we show that single ultrafast coherent x-ray pulses can be used to observe the speckle contrast in the high-angle diffraction from liquid Ga and glassy Ni2Pd2P and B2O3. We determine the thresholds above which the x-ray pulses disturb the atomic arrangements. Furthermore, high contrast speckle is observed in scattering patterns from the glasses integrated over many pulses, demonstrating that the source and optics are sufficiently stable for x-ray photon correlation spectroscopy studies of dynamics over a wide range of time scales.
Crystallographic imperfections significantly alter material properties and their response to external stimuli, including solute-induced phase transformations. Despite recent progress in imaging defects using electron and X-ray techniques, in situ three-dimensional imaging of defect dynamics remains challenging. Here, we use Bragg coherent diffractive imaging to image defects during the hydriding phase transformation of palladium nanocrystals. During constant-pressure experiments we observe that the phase transformation begins after dislocation nucleation close to the phase boundary in particles larger than 300 nm. The three-dimensional phase morphology suggests that the hydrogen-rich phase is more similar to a spherical cap on the hydrogen-poor phase than to the core-shell model commonly assumed. We substantiate this using three-dimensional phase field modelling, demonstrating how phase morphology affects the critical size for dislocation nucleation. Our results reveal how particle size and phase morphology affects transformations in the PdH system.
We imaged nanoscale lattice strain in a multilayer semiconductor device prototype with a new X-ray technique, nanofocused Bragg projection ptychography. Applying this technique to the epitaxial stressor layer of a SiGe-on-SOI structure, we measured the internal lattice behavior in a targeted region of a single device and demonstrated that its internal strain profile consisted of two competing lattice distortions. These results provide the strongest nondestructive test to date of continuum modeling predictions of nanoscale strain distributions.
We present an efficient method of imaging 3D nanoscale lattice behavior and strain fields in crystalline materials with a new methodology -three dimensional Bragg projection ptychography (3DBPP). In this method, the 2D sample structure information encoded in a coherent high-angle Bragg peak measured at a fixed angle is combined with the real-space scanning probe positions to reconstruct the 3D sample structure. This work introduces an entirely new means of three dimensional structural imaging of nanoscale materials and eliminates the experimental complexities associated with rotating nanoscale samples. We present the framework for the method and demonstrate our approach with a numerical demonstration, an analytical derivation, and an experimental reconstruction of lattice distortions in a component of a nanoelectronic prototype device.Inversion methods provide a powerful alternative to traditional objective-lens-based microscopy. Techniques that numerically invert coherent diffraction patterns into real space images have provided substantial gains in resolution and sensitivity in certain optical, electron, and x-ray microscopy experiments, especially where image-forming lenses are inefficient or difficult to incorporate. The resulting images, formed by inverting reciprocal space diffraction patterns, contain quantitative information that encodes local physical parameters such as permittivity, density, and atomic displacement at sub-beam-size spatial resolutions.When implemented with hard x-rays, these coherent diffraction imaging (CDI) techniques have enhanced our understanding of the internal structure of nano-and meso-scale materials, especially in operating environments that are difficult to access with other probes. Furthermore, x-ray microscopy methods based on Bragg diffraction are of particular interest because the sensitivity of x-rays to crystalline distortions in materials can be leveraged to reveal the interplay between structure and properties without disturbing environmental boundary conditions. However, the routine application of inversion methods to coherent hard x-ray Bragg diffraction is still limited by stringent experimental requirements and long measurement times.Given the potential impact of non-destructive 3D structural microscopy and the limitations of current 3D Bragg coherent x-ray inversion methods, advances in Bragg phase retrieval methods that facilitate the rapid imaging of crystal lattice behavior in realistic environments are critically important. Here, we introduce a new coherent Bragg diffraction imaging approach, three dimensional Bragg projection ptychography (3DBPP), that provides such a capability. 3DBPP enables 3D image reconstruction from a series of 2D Bragg diffraction patterns measured at a single incident beam angle, thus forming a new mode of inversion-based 3D strain-sensitive imaging. As we discuss in this article, 3DBPP is a hybrid real / reciprocal space technique that takes advantage of the high angle of separation between the incident and diffracted beam in a Bra...
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