Scanning Coherent Diffraction Imaging Research Articles

Fast and efficient hard X-ray projection imaging below 10 nm resolution.

High-resolution X-ray imaging of noncrystalline objects is often achieved through the approach of scanning coherent diffractive imaging known as ptychography. The imaging resolution is usually limited by the scattering properties of the sample, where weak diffraction signals at the highest scattering angles compete with parasitic scattering. Here, we demonstrate that X-ray multilayer Laue lenses with a high numerical aperture (NA) can be used to create a strong reference beam that holographically boosts weak scattering from the sample over a large range of scattering angles, enabling high-resolution imaging that is tolerant of such background. An imaging resolution of sub-10 nm was achieved at a photon energy of 17.4 keV with lenses of 0.014 NA from a Siemens star test object and a sample of hierarchical nanoporous gold, recording projection holograms at an effective magnification of more than 30,000 directly on a pixel-array detector. A numerical study compared this approach to low-NA far-field ptychography, indicating significant advantages for using high-NA lenses in the presence of background noise. This imaging modality is particularly fast and efficient at recording high-resolution transmission phase-contrast images over large fields of view in a facile manner.

Fast X-ray ptychography: towards nanoscale imaging of large volume of brain

X-ray ptychography, a scanning coherent diffraction imaging technique, is one of the most used techniques at synchrotron facilities for high resolution imaging, with applications spanning from life science to nano-electronics. In the recent years there has been a great effort to make the technique faster to enable high throughput nanoscale imaging. Here we apply a fast ptychography scanning method to image in 3D 106μm3\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$10^6\\upmu \\mathrm{{m}}^3$$\\end{document} of brain-like phantom at 3 kHz, in a 7 h acquisition with a resolution of 270 nm. We then present the latest advances in fast ptychography by showing 2D images acquired at 110 kHz by combining the fast-acquisition scheme with a high-acquisition rate prototype detector from DECTRIS Ltd. We finally review the experimental outcome and discuss the prospective use of fast ptychography schemes for the investigation of mm3\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$^{3}$$\\end{document} size samples of brain-like phantom, by extrapolating the current results to the high coherent flux scenario of diffraction limited storage rings.

Quantitative, in situ visualization of intracellular insulin vesicles in pancreatic beta cells

Characterizing relationships between Zn2+, insulin, and insulin vesicles is of vital importance to the study of pancreatic beta cells. However, the precise content of Zn2+ and the specific location of insulin inside insulin vesicles are not clear, which hinders a thorough understanding of the insulin secretion process and diseases caused by blood sugar dysregulation. Here, we demonstrated the colocalization of Zn2+ and insulin in both single extracellular insulin vesicles and pancreatic beta cells by using an X-ray scanning coherent diffraction imaging (ptychography) technique. We also analyzed the elemental Zn2+ and Ca2+ contents of insulin vesicles using electron microscopy and energy dispersive spectroscopy (EDS) mapping. We found that the presence of Zn2+ is an important characteristic that can be used to distinguish insulin vesicles from other types of vesicles in pancreatic beta cells and that the content of Zn2+ is proportional to the size of insulin vesicles. By using dual-energy contrast X-ray microscopy and scanning transmission X-ray microscopy (STXM) image stacks, we observed that insulin accumulates in the off-center position of extracellular insulin vesicles. Furthermore, the spatial distribution of insulin vesicles and their colocalization with other organelles inside pancreatic beta cells were demonstrated using three-dimensional (3D) imaging by combining X-ray ptychography and an equally sloped tomography (EST) algorithm. This study describes a powerful method to univocally describe the location and quantitative analysis of intracellular insulin, which will be of great significance to the study of diabetes and other blood sugar diseases.

Flexible ptychography platform to expand the potential of imaging at free electron lasers.

Ptychography, a scanning coherent diffraction imaging method, can produce a high-resolution reconstruction of a sample and, at the same time, of the illuminating beam. The emergence of vacuum ultraviolet and X-ray free electron lasers (FELs) has brought sources with unprecedented characteristics that enable X-ray ptychography with highly intense and ultra-fast short-wavelength pulses. However, the shot-to-shot pulse fluctuations typical for FEL pulses and particularly the partial spatial coherence of self-amplified spontaneous emission (SASE) FELs lead to numerical complexities in the ptychographic algorithms and ultimately restrict the application of ptychography at FELs. We present a general adaptive forward model for ptychography based on automatic differentiation, which is able to perform reconstructions even under these conditions. We applied this model to the first ptychography experiment at FLASH, the Free electron LASer in Hamburg, and obtained a high-resolution reconstruction of the sample as well as the complex wavefronts of individual FLASH pulses together with their coherence properties. This is not possible with more common ptychography algorithms.

Nanoscale Detection of Subcellular Nanoparticles by X-Ray Diffraction Imaging for Precise Quantitative Analysis of Whole Cancer Cells.

Nanoparticles show great potential for drug delivery systems in cancer treatment and diagnosis, which mainly rely on the interaction between nanoparticles and living cells. However, there is still a lack of accurate and large field-of-view imaging techniques to reveal the aggregation and distribution behavior of nanoparticles in whole cancer cells without being destroyed. Here, we demonstrated quantitative imaging of unstained and intact mouse breast cancer cells (4T1) containing 50 nm gold nanoparticles (Au@citrate NPs) using an X-ray scanning coherent diffraction imaging (ptychography) technique in a large field-of-view. A two-dimensional spatial resolution of 17 nm was achieved on the 4T1 cell. We combine X-ray ptychography and equally sloped tomography (EST) to perform three-dimensional structural mapping, distribution, and aggregation behavior of Au@citrate NPs in cancer cells. By taking full advantage of the large field-of-view, high-resolution, and quantitative imaging technique, the single intracellular Au@citrate NPs are observed and the amount of Au@citrate NPs in aggregations can be accurately quantified. In addition, the morphological changes of lysosomes containing Au@citrate NPs can be observed in the high-contrast mass density images. This study provides an approach for exploring quantitative analysis and physiological delivery of nanomaterials in intact cancer cells at nanoscale resolution, which may greatly benefit the interdisciplinary research of material science, nanomedicine, and nanotoxicology.

Aberration characterization of x-ray optics using multi-modal ptychography and a partially coherent source

Ptychography is a scanning coherent diffraction imaging technique that provides high-resolution imaging and complete spatial information of the complex probe and object transmission function. The wavefront error caused by aberrated optics has previously been recovered using ptychography when a highly coherent source is used, but has not been demonstrated with partial coherence due to the multi-modal probe required. Here, we demonstrate that partial coherence can be accounted for in ptychographic reconstructions using the multi-modal approach and assuming that decoherence arises from either the probe or the object. This equivalence recovers coherent (or single state) reconstructions of both the probe and the object even in the presence of partial coherence. We demonstrate this experimentally by using hard x-ray ptychography with a partially coherent source to image a Siemens star test object and to also recover the wavefront error from an aberrated beryllium compound refractive lens. The source properties and resolving capabilities are analyzed, and the wavefront error results are compared with another at-wavelength metrology technique. Our work demonstrates the capability of ptychography to provide high-resolution imaging and optics characterization even in the presence of partial coherence.

Hard X-ray ptychography for optics characterization using a partially coherent synchrotron source.

Ptychography is a scanning coherent diffraction imaging technique which provides high resolution imaging and complete spatial information of the complex electric field probe and sample transmission function. Its ability to accurately determine the illumination probe has led to its use at modern synchrotrons and free-electron lasers as a wavefront-sensing technique for optics alignment, monitoring and correction. Recent developments in the ptychography reconstruction process now incorporate a modal decomposition of the illuminating probe and relax the restriction of using sources with high spatial coherence. In this article a practical implementation of hard X-ray ptychography from a partially coherent X-ray source with a large number of modes is demonstrated experimentally. A strongly diffracting Siemens star test sample is imaged using the focused beam produced by either a Fresnel zone plate or beryllium compound refractive lens. The recovered probe from each optic is back propagated in order to plot the beam caustic and determine the precise focal size and position. The power distribution of the reconstructed probe modes also allows the quantification of the beams coherence and is compared with the values predicted by a Gaussian-Schell model and the optics exit intensity.

Ptychography at the Linac Coherent Light Source in a parasitic geometry

X-ray free-electron lasers (FELs) are being recognized as a powerful tool in an ever-increasing number of research fields, but are very limited as to the number of experiments that they can support. This work shows that more beamtime could be made available by using `parasitic' geometries, where a secondary experiment uses the X-ray beam that the primary experiment does not utilize. The first successful ptychography experiment, a scanning coherent diffractive imaging technique, in a parasitic geometry at an X-ray FEL is demonstrated. Utilizing the CXI hutch at the Linac Coherent Light Source (LCLS), it is shown that the obtained data are of high quality and that characterizing the beam using ptychography can be much faster than traditional imprinting methods.

AI-enabled high-resolution scanning coherent diffraction imaging

Ptychographic imaging is a powerful means of imaging beyond the resolution limits of typical x-ray optics. Recovering images from raw ptychographic data, however, requires the solution of an inverse problem, namely, phase retrieval. Phase retrieval algorithms are computationally expensive, which precludes real-time imaging. In this work, we propose PtychoNN, an approach to solve the ptychography data inversion problem based on a deep convolutional neural network. We demonstrate how the proposed method can be used to predict real-space structure and phase at each scan point solely from the corresponding far-field diffraction data. Our results demonstrate the practical application of machine learning to recover high fidelity amplitude and phase contrast images of a real sample hundreds of times faster than current ptychography reconstruction packages. Furthermore, by overcoming the constraints of iterative model-based methods, we can significantly relax sampling constraints on data acquisition while still producing an excellent image of the sample. Besides drastically accelerating acquisition and analysis, this capability has profound implications for the imaging of dose sensitive, dynamic, and extremely voluminous samples.

Correlative XRF, ptychography and light microscopy on shielding pigments of Clunio larval ocelli

The nature of retinal shielding pigment in the larval eyes of the midge Clunio marinus was studied by high resolution scanning X-ray fluorescence (XRF) analysis correlated with light microscopy (LM) and scanning coherent X-ray diffractive imaging (ptychography). Clunio is known as a unique model system to decipher mechanisms underlying the complex moon-related rhythms. Shielding pigment granules within the photoreceptor cells of their primitive eyes (ocelli) have been shown to change appearance in the same rhythm. We compared the relative amount of trace metals (Ca, Ni, Zn, Cu), obtained by XRF, within single melanosomes (diameter about 500 nm) and the surrounding photoreceptor cells with their optical density in the light microscope and—for the first time—the electron density derived from ptychography images. Though individual pigment granules can be identified and correlated in images of all three techniques the optical density, electron density and especially element concentrations within individual granules seem to vary independently. We discuss that the state of melanogenesis is not synchronized inside the ocellus.

High-Resolution Imaging of Polymer Electrolyte Membrane Fuel Cell Cathode Layers by Soft X-ray Spectro-Ptychography

Polymer electrolyte membrane fuel cells (PEMFCs) are a promising and sustainable alternative to internal combustion engines for automotive applications. Polymeric perfluorosulfonic acid (PFSA) plays a key role in PEMFCs as a proton conductor in the anode and cathode catalyst layers and in the electrolyte membrane. In this study, spectroscopic scanning coherent diffraction imaging (spectro-ptychography) and spectro-ptychographic tomography were used to quantitatively image PFSA ionomers in PEMFC cathodes in both two and three dimensions. We verify that soft X-ray ptychography gives significant spatial resolution improvement on soft matter polymeric materials. A two-dimensional spatial resolution of better than 15 nm was achieved. With better detectors and brighter and more coherent X-ray beams, radiation-sensitive PFSA ionomers will be visualized with acceptable levels of chemical and structural modification. This work is a step toward visualization of ionomers in PEMFC cathodes at high spatial resolution ...

Ptychographic imaging with partially coherent plasma EUV sources

Abstract We report on high-resolution lens-less imaging experiments based on ptychographic scanning coherent diffractive imaging (CDI) method employing compact plasma sources developed for extreme ultraviolet (EUV) lithography applications. Two kinds of discharge sources were used in our experiments: a hollow-cathode-triggered pinch plasma source operated with oxygen and for the first time a laser-assisted discharge EUV source with a liquid tin target. Ptychographic reconstructions of different samples were achieved by applying constraint relaxation to the algorithm. Our ptychography algorithms can handle low spatial coherence and broadband illumination as well as compensate for the residual background due to plasma radiation in the visible spectral range. Image resolution down to 100 nm is demonstrated even for sparse objects, and it is limited presently by the sample structure contrast and the available coherent photon flux. We could extract material properties by the reconstruction of the complex exit-wave field, gaining additional information compared to electron microscopy or CDI with longer-wavelength high harmonic laser sources. Our results show that compact plasma-based EUV light sources of only partial spatial and temporal coherence can be effectively used for lens-less imaging applications. The reported methods may be applied in combination with reflectometry and scatterometry for high-resolution EUV metrology.

Ptychographic reconstruction algorithm for frequency-resolved optical gating: super-resolution and supreme robustness

Frequency-resolved optical gating (FROG) is probably the most popular technique for complete characterization of ultrashort laser pulses. In FROG, a reconstruction algorithm retrieves the pulse from a measured spectrogram, yet current FROG reconstruction algorithms require and exhibit several restricting features that weaken FROG performances. For example, the delay step must correspond to the spectral bandwidth measured with large enough SNR a condition that limits the temporal resolution of the reconstructed pulse, obscures measurements of weak broadband pulses, and makes measurement of broadband mid-IR pulses hard and slow because the spectrograms become huge. We develop a new approach for FROG reconstruction, based on ptychography (a scanning coherent diffraction imaging technique), that removes many of the algorithmic restrictions. The ptychographic reconstruction algorithm is significantly faster and more robust to noise than current FROG algorithms, which are based on generalized projections (GP). We demonstrate, numerically and experimentally, that ptychographic reconstruction works well with very partial spectrograms, e. g. spectrograms with reduced number of measured delays and spectrograms that have been substantially spectrally filtered. In addition, we implement the ptychogrpahic approach to blind second harmonic generation (SHG) FROG and demonstrate robust and complete characterization of two unknown pulses from a single measured spectrogram and power spectrum of only one of the pulses. We believe that the ptychograpy-based approach will become the standard reconstruction procedure in FROG and related diagnostics methods, allowing successful reconstructions from so far unreconstructable spectrograms.

Scanning coherent diffractive imaging methods for actinic extreme ultraviolet mask metrology

For the successful implementation of extreme ultraviolet (EUV) lithography in the upcoming technology nodes, a major challenge to overcome is the stable and reliable detection and characterization of mask defects. We have recently presented a reflective mode EUV mask scanning lensless imaging tool (RESCAN) which was installed at the XIL-II beamline of the swiss light source and showed reconstructed aerial images of test patterns on EUV masks. RESCAN uses scanning coherent diffractive imaging (SCDI) methods to obtain actinic aerial images of EUV photomasks and was designed for 80 nm onmask resolution. Our SCDI algorithm reconstructs the measured sample by iteratively solving the phase problem using overdetermined diffraction data gathered by scanning across the specimen with a finite illumination. It provides the phase and amplitude aerial images of EUV photomasks with high resolution without the need to use high numerical aperture (NA) lenses. Contrary to scanning microscopy and full-field microscopy, where the resolution is limited by the spot size or NA of the lens, the achievable resolution with our method depends on the detector noise and NA of the detector. To increase the resolution of our tool, we upgraded RESCAN with a detector and algorithms. Here, we present the results obtained with the tool that is capable of up to 40-nm onmask resolution. We believe that the realization of our prototype marks a significant step toward overcoming the limitations imposed by methods relying on imaging optics and shows a viable solution for actinic mask metrology.

Ptychographic coherent diffractive imaging with orthogonal probe relaxation.

Ptychography is a scanning coherent diffractive imaging (CDI) technique that relies upon a high level of stability of the illumination during the course of an experiment. This is particularly an issue for coherent short wavelength sources, where the beam intensity is usually tightly focused on the sample in order to maximize the photon flux density on the illuminated region of the sample and thus a small change in the beam position results in a significant change in illumination of the sample. We present an improved ptychographic method that allows for limited stability of the illumination wavefront and thus significantly improve the reconstruction quality without additional prior knowledge. We have tested our reconstruction method in a proof of concept experiment, where the beam instability of a visible light source was emulated using a piezo driven mirror, and also in a short wavelength microscopy CDI setup using a high harmonic generation source in the extreme ultraviolet range. Our work shows a natural extension of the ptychography method that paves the way to use ptychographic imaging with any limited pointing stability coherent source such as free electron or soft X-ray lasers and improve reconstruction quality of long duration synchrotron experiments.

基于光学相干层析成像的视网膜图像自动分层方法

Ptychography, a phase retrieval technology based on scanning coherent diffractive imaging, shows such advantages as simple experimental setup and strong anti-noise ability. Ptychography is used in the field of wavefront metrology for projection lens. The formulas of optical field propagation, the conditions of discretion, and the experimental configurations are analyzed in detail for projection lenses with different numerical apertures. Numerical simulations and experimental results show that to achieve reasonable convergence and measurement accuracy, the transmittance of the object should be set between 45% and 80%. Increasing the complexity of the object pattern and adding registration process of probe and object into the iterative algorithm can also improve the convergence speed and the recovery accuracy. The wavefront aberration measurement accuracy can reach 10~(-3)lambda or less. It is feasible to use ptychography in wavefront aberration measurement for extreme ultraviolet lithographic projection lenses.

Influence of finite spatial coherence on ptychographic reconstruction

X-ray ptychography is an ultrahigh-resolution scanning coherent diffractive imaging technique, allowing quantitative measurements of extended samples and a simultaneous reconstruction of the illuminating wavefront. Recent development of the mixed-state reconstruction algorithm has triggered a certain interest in utilizing partially coherent X-ray sources for ptychography. Here, we study how finite spatial coherence influences the reconstructed image of a test structure. Our work shows that use of a highly coherent illumination provides images with better spatial resolution and fewer artefacts than the approach with partial coherence.

Coherent imaging at the diffraction limit.

X-ray ptychography, a scanning coherent diffractive imaging technique, holds promise for imaging with dose-limited resolution and sensitivity. If the foreseen increase of coherent flux by orders of magnitude can be matched by additional technological and analytical advances, ptychography may approach imaging speeds familiar from full-field methods while retaining its inherently quantitative nature and metrological versatility. Beyond promises of high throughput, spectroscopic applications in three dimensions become feasible, as do measurements of sample dynamics through time-resolved imaging or careful characterization of decoherence effects.

Ptychography with broad-bandwidth radiation

Ptychography, a scanning Coherent Diffractive Imaging (CDI) technique, has quickly gained momentum as a robust method to deliver quantitative images of extended specimens. A current conundrum for the development of X-ray CDI is the conflict between a need for higher flux to reach higher resolutions and the requirement to strongly filter the incident beam to satisfy the tight coherence prerequisite of the technique. Latest developments in algorithmic treatment of ptychographic data indicate that the technique is more robust than initially assumed, so that some experimental limitations can be substantially relaxed. Here, we demonstrate that ptychography can be conducted in conditions that were up to now considered insufficient, using a broad-bandwidth X-ray beam and an integrating scintillator-based detector. Our work shows the wide applicability of ptychography and paves the way to high-throughput, high-flux diffractive imaging.

Observations of artefacts in the x-ray ptychography method.

X-ray ptychography, a scanning coherent diffraction imaging method, was used to reconstruct images of a "Siemens star" test pattern with amplitude and phase contrast. While studying how the use of illumination with an increased bandwidth results in clear improvements in the quality of image reconstructions, we found that an artificial change in the overall distance scale factor of the algorithm leads to a systematic response in the image, which is reproduced with an incorrect number of spokes. This pathology is explained by the conflict between the length scales set by the scan and by the diffraction patterns on the detector.