X-ray ptychographic and fluorescence microscopy using virtual single-pixel imaging based deconvolution with accurate probe images.

Simultaneous measurement of X-ray ptychography and fluorescence microscopy allows high-resolution and high-sensitivity observations of the microstructure and trace-element distribution of a sample. In this paper, we propose a method for improving scanning fluorescence X-ray microscopy (SFXM) images, in which the SFXM image is deconvolved via virtual single-pixel imaging using different probe images for each scanning point obtained by X-ray ptychographic reconstruction. Numerical simulations confirmed that this method can increase the spatial resolution while suppressing artifacts caused by probe imprecision, e.g., probe position errors and wavefront changes. The method also worked well in synchrotron radiation experiments to increase the spatial resolution and was applied to the observation of S element maps of ZnS particles.

High-resolution and high-sensitivity X-ray ptychographic coherent diffraction imaging using the CITIUS detector.

Ptychographic coherent diffraction imaging (PCDI) is a synchrotron X-ray microscopy technique that provides high spatial resolution and a wide field of view. To improve the performance of PCDI, the performance of the synchrotron radiation source and imaging detector should be improved. In this study, ptychographic diffraction pattern measurements using the CITIUS high-speed X-ray image detector and the corresponding image reconstruction are reported. X-rays with an energy of 6.5 keV were focused by total reflection focusing mirrors, and a flux of ∼2.6 × 1010 photons s-1 was obtained at the sample plane. Diffraction intensity data were collected at up to ∼250 Mcounts s-1 pixel-1 without saturation of the detector. Measurements of tantalum test charts and silica particles and the reconstruction of phase images were performed. A resolution of ∼10 nm and a phase sensitivity of ∼0.01 rad were obtained. The CITIUS detector can be applied to the PCDI observation of various samples using low-emittance synchrotron radiation sources and to the stability evaluation of light sources.

Nanoscale domain imaging of Li-rich disordered rocksalt-type cathode materials with X-ray spectroscopic ptychography.

Lithium-rich disordered rocksalt-type cathode materials are promising for high-capacity and high-power lithium-ion batteries. Many of them are synthesized by mechanical milling and may have heterogeneous structures and chemical states at the nanoscale. In this study, we performed X-ray spectroscopic ptychography measurements of Li-rich disordered rocksalt-type oxide particles synthesized by mechanical milling before and after delithiation reaction at the vanadium K absorption edge, and visualized their structures and chemical state with a spatial resolution of ∼100 nm. We classified multiple domains with different chemical states via clustering analysis. A comparison of the domain distribution trends of the particles before and after the delithiation reaction revealed the presence of domains, suggesting that the delithiation reaction was suppressed.

Visualization of Structural Heterogeneities in Particles of Lithium Nickel Manganese Oxide Cathode Materials by Ptychographic X-ray Absorption Fine Structure.

A heterogeneous phase/structure distribution in the bulk of spinel lithium nickel manganese oxides (LNMOs) is the key to maximizing the performance and stability of the cathode materials of lithium-ion batteries. Herein, we report the use of two-dimensional ptychographic X-ray absorption fine structure (XAFS) to visualize the density and valence maps of manganese and nickel in as-prepared LNMO particles and unsupervised learning to classify the three-phase group in terms of different elemental compositions and chemical states. The described approach may increase the supply of information for nanoscale characterization and promote the design of suitable structural domains to maximize the performance and stability of batteries.

Demonstration of single-frame coherent X-ray diffraction imaging using triangular aperture: Towards dynamic nanoimaging of extended objects.

Coherent diffraction imaging (CDI) is a powerful method for visualizing the structure of an object with a high spatial resolution that exceeds the performance limits of the lens. Single-frame CDI in the X-ray region has potential use for probing dynamic phenomena with a high spatiotemporal resolution. Here, we experimentally demonstrate a general method for single-frame X-ray CDI using a triangular aperture and a Fresnel zone plate. Using 5 keV synchrotron radiation X-rays, we reconstructed the object image of the locally illuminated area with a spatial resolution of higher than 50 nm and an exposure time of more than 0.1 s without prior information about the sample. After a 10 s exposure, a resolution of 17 nm was achieved. The present method opens new frontiers in the study of dynamics at the nanoscale by using next-generation synchrotron radiation X-rays/free-electron lasers as light sources.

Single-frame coherent diffraction imaging of extended objects using triangular aperture.

We propose a method of single-frame coherent diffraction imaging using a triangular aperture, which can not only reconstruct the projection image of extended objects from a single-frame coherent diffraction pattern, but also improve the image of the wavefield of the probe. In this method, a plane-wave illuminates a triangular aperture. An object is placed immediately after the aperture or in the image plane of the aperture through a lens. A far-field coherent diffraction pattern is collected by a two-dimensional detector. The object image is reconstructed from the single-frame diffraction pattern using a phase retrieval algorithm without support constraints. We simulate feasible experimental setups in the hard X-ray regime and show that this method can be practical use for single-frame coherent diffraction imaging. The present method has the potential exploring dynamic phenomena in materials science and biology with high spatiotemporal resolution using synchrotron radiation/free-electron lasers.