Transmission electron microscopes use electrons with wavelengths of a few picometers, potentially capable of imaging individual atoms in solids at a resolution ultimately set by the intrinsic size of ...an atom. However, owing to lens aberrations and multiple scattering of electrons in the sample, the image resolution is reduced by a factor of 3 to 10. By inversely solving the multiple scattering problem and overcoming the electron-probe aberrations using electron ptychography, we demonstrate an instrumental blurring of less than 20 picometers and a linear phase response in thick samples. The measured widths of atomic columns are limited by thermal fluctuations of the atoms. Our method is also capable of locating embedded atomic dopant atoms in all three dimensions with subnanometer precision from only a single projection measurement.
Understanding and control of the dynamic response of magnetic materials with a three-dimensional magnetization distribution is important both fundamentally and for technological applications. From a ...fundamental point of view, the internal magnetic structure and dynamics in bulk materials still need to be mapped
, including the dynamic properties of topological structures such as vortices
, magnetic singularities
or skyrmion lattices
. From a technological point of view, the response of inductive materials to magnetic fields and spin-polarized currents is essential for magnetic sensors and data storage devices
. Here, we demonstrate time-resolved magnetic laminography, a pump-probe technique, which offers access to the temporal evolution of a three-dimensional magnetic microdisc with nanoscale resolution, and with a synchrotron-limited temporal resolution of 70 ps. We image the dynamic response to a 500 MHz magnetic field of the complex three-dimensional magnetization in a two-phase bulk magnet with a lateral spatial resolution of 50 nm. This is achieved with a stroboscopic measurement consisting of eight time steps evenly spaced over 2 ns. These measurements map the spatial transition between domain wall motion and the dynamics of a uniform magnetic domain that is attributed to variations in the magnetization state across the phase boundary. Our technique, which probes three-dimensional magnetic structures with temporal resolution, enables the experimental investigation of functionalities arising from dynamic phenomena in bulk and three-dimensional patterned nanomagnets
.
Over the past decade, ptychography has been proven to be a robust tool for non‐destructive high‐resolution quantitative electron, X‐ray and optical microscopy. It allows for quantitative ...reconstruction of the specimen's transmissivity, as well as recovery of the illuminating wavefront. Additionally, various algorithms have been developed to account for systematic errors and improved convergence. With fast ptychographic microscopes and more advanced algorithms, both the complexity of the reconstruction task and the data volume increase significantly. PtychoShelves is a software package which combines high‐level modularity for easy and fast changes to the data‐processing pipeline, and high‐performance computing on CPUs and GPUs.
A new computer program for analysing ptychographic data combines both high‐level simplicity and high‐performance computing on large‐scale computing clusters. It is available with a royalty‐free non‐exclusive licence for academic and non‐commercial purposes.
Although ptychography does not require a precise knowledge of the illumination wavefront, common implementations rely upon assumptions such as accurate knowledge of the scan positions and constant ...illumination. Limited validity of these assumptions results in deterioration of the reconstruction quality. We present a generalized ptychography method that optimizes the reconstruction along multiple directions. In our manuscript, we demonstrate that the additional flexibility not only helps to amend imprecisions of the ptychography model in a self-consistent way but additionally leads to faster convergence without a significant increase of the computational cost per iteration.
We present a systematic study, where effects of the illumination probe design on ptychography reconstruction quality are evaluated under well-controlled conditions. The illumination probe was created ...using Fresnel zone-plate (FZP) optics with locally displaced zones to provide a fine control over perturbations of the illumination wavefront. We show that optimally designed wavefront modulations not only reduce bias and variance in the reconstruction of the lowest spatial frequencies but also lead to improved imaging resolution and reduction of artefacts compared to a conventional FZP. Both these factors are important for quantitative accuracy and resolution of ptychographic tomography. Our work furthers the understanding of the important characteristics of an optimal illumination for high-resolution X-ray ptychography and how to design optimal FZP wavefront modulations for different applications of ptychographic imaging. These findings are applicable and relevant for ptychography using optical, EUV, and X-ray photons as well as electrons.
The search for higher performance, improved safety, and lifetime of lithium-ion batteries relies on the understanding of degradation mechanisms. Complementary to methods and studies on primary ...particles or crystalline structure on bulk materials, here we use spatially correlated ptychographic X-ray computed nanotomography with a 35 nm resolution and scanning X-ray diffraction microscopy with 1 μm resolution to visualize in 3D the hidden morphological and structural degradation processes in individual secondary particles of lithium-rich nickel, cobalt, and manganese oxides. From comparative examination of pristine and cycled particles, we suggest that morphological degradation could have radial dependency and secondary particle size dependency. The same particles were examined to correlate the degradation to crystallinity, which shows surprising core-shell structures. This study reveals the inner 3D structure of the secondary particles while opening up questions on the unexpected crystalline structural distributions, which could offer clues for future studies on this promising cathode material for lithium-ion batteries.
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•Correlative ptychographic tomography with 35 nm resolution and diffraction tomography•3D micro-cracks in secondary Li-rich NMC particles correlated with crystal lattice•Radial and secondary-particle-size-dependent material degradation•Intriguing core-shell structure observed in 3D crystalline maps
Materials Characterization Techniques; Energy Materials; Crystallography
Ptychography is a coherent diffractive imaging method that can provide a diffraction-limited, robust reconstruction of the sample's complex transmission function without the use of high-quality ...optics. However, the scanning nature of conventional X-ray ptychography unavoidably requires the mechanical motion of either the illumination probe or the sample. In order to avoid overhead related to breaking and acceleration for every scan position, so-called fly-scan methods were developed. Here, we present an improved variant that removes the limitation of continuous scanning along a linear scanning path and allows for ptychographic reconstruction of scans taken along an arbitrary 2D continuous trajectory. We also demonstrate numerically and experimentally that our method provides significantly improved robustness against noise, particularly for larger fly-scan steps, i.e. sample shift during an exposure, which will gain importance with the advent of 4th generation synchrotron sources, where the available coherent flux may be increased by orders of magnitude. Finally, we show that the use of a spiral scan continuous trajectory alleviates significantly raster grid artifacts.
As the resolution of X-ray tomography improves, the limited long-term stability and accuracy of nanoimaging tools does not allow computing artifact-free three-dimensional (3D) reconstructions without ...an additional step of numerical alignment of the measured projections. However, the common iterative alignment methods are significantly more computationally demanding than a simple tomographic reconstruction of the acquired volume. Here, we address this issue and present an alignment toolkit, which exploits methods with deep-subpixel accuracy combined with a multi-resolution scheme. This leads to robust and accurate alignment with significantly reduced computational and memory requirements. The performance of the presented methods is demonstrated on simulated and measured datasets for tomography and also laminography acquisition geometries. A GPU accelerated implementation of our alignment framework is publicly available.
The COMPASS tokamak is equipped with the soft X-ray (SXR) diagnostic system based on silicon photodiode arrays shielded by a thin beryllium foil. The diagnostic is composed of two pinhole cameras ...having 35 channels each and one vertical pinhole camera with 20 channels, which was installed recently to improve tomographic inversions. Lines of sight of the SXR detectors cover almost complete poloidal cross section of the COMPASS vessel with a spatial resolution of 1-2 cm and temporal resolution of about 3 μs. Local emissivity is reconstructed via Tikhonov regularization constrained by minimum Fisher information that provides reliable and robust solution despite limited number of projections and ill-conditionality of this task. Improved border conditions and numerical differentiation matrices suppressing artifacts in reconstructed radiation were implemented in the code. Furthermore, a fast algorithm eliminating iterative processes was developed, and it is foreseen to be tested in real-time plasma control.
Both high resolution and high precision are required to quantitatively determine the atomic structure of complex nanostructured materials. However, for conventional imaging methods in scanning ...transmission electron microscopy (STEM), atomic resolution with picometer precision cannot usually be achieved for weakly-scattering samples or radiation-sensitive materials, such as 2D materials. Here, we demonstrate low-dose, sub-angstrom resolution imaging with picometer precision using mixed-state electron ptychography. We show that correctly accounting for the partial coherence of the electron beam is a prerequisite for high-quality structural reconstructions due to the intrinsic partial coherence of the electron beam. The mixed-state reconstruction gains importance especially when simultaneously pursuing high resolution, high precision and large field-of-view imaging. Compared with conventional atomic-resolution STEM imaging techniques, the mixed-state ptychographic approach simultaneously provides a four-times-faster acquisition, with double the information limit at the same dose, or up to a fifty-fold reduction in dose at the same resolution.
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