Scanning WAXS microscopy of regenerated cellulose fibers at mesoscopic resolution.

In this work, regenerated cellulose textile fibers, Ioncell-F, dry-wet spun with different draw ratios, have been investigated by scanning wide-angle X-ray scattering (WAXS) using a mesoscopic X-ray beam. The fibers were found to be homogeneous on the 500 nm length scale. Analysis of the azimuthal angular dependence of a crystalline Bragg spot intensity revealed a radial dependence of the degree of orientation of crystallites that was found to increase with the distance from the center of the fiber. We attribute this to radial velocity gradients during the extrusion of the spin dope and the early stage of drawing. On the other hand, the fiber crystallinity was found to be essentially homogeneous over the fiber cross section.

Deep learning approach for denoising low-SNR correlation plenoptic images.

Correlation Plenoptic Imaging (CPI) is a novel volumetric imaging technique that uses two sensors and the spatio-temporal correlations of light to detect both the spatial distribution and the direction of light. This novel approach to plenoptic imaging enables refocusing and 3D imaging with significant enhancement of both resolution and depth of field. However, CPI is generally slower than conventional approaches due to the need to acquire sufficient statistics for measuring correlations with an acceptable signal-to-noise ratio (SNR). We address this issue by implementing a Deep Learning application to improve image quality with undersampled frame statistics. We employ a set of experimental images reconstructed by a standard CPI architecture, at three different sampling ratios, and use it to feed a CNN model pre-trained through the transfer learning paradigm U-Net architecture with VGG-19 net for the encoding part. We find that our model reaches a Structural Similarity (SSIM) index value close to 1 both for the test sample (SSIM = [Formula: see text]) and in 5-fold cross validation (SSIM = [Formula: see text]); the results are also shown to outperform classic denoising methods, in particular for images with lower SNR. The proposed work represents the first application of Artificial Intelligence in the field of CPI and demonstrates its high potential: speeding-up the acquisition by a factor 20 over the fastest CPI so far demonstrated, enabling recording potentially 200 volumetric images per second. The presented results open the way to scanning-free real-time volumetric imaging at video rate, which is expected to achieve a substantial influence in various applications scenarios, from monitoring neuronal activity to machine vision and security.

Correlated-photon imaging at 10 volumetric images per second.

The correlation properties of light provide an outstanding tool to overcome the limitations of traditional imaging techniques. A relevant case is represented by correlation plenoptic imaging (CPI), a quantum-inspired volumetric imaging protocol employing spatio-temporally correlated photons from either entangled or chaotic sources to address the main limitations of conventional light-field imaging, namely, the poor spatial resolution and the reduced change of perspective for 3D imaging. However, the application potential of high-resolution imaging modalities relying on photon correlations is limited, in practice, by the need to collect a large number of frames. This creates a gap, unacceptable for many relevant tasks, between the time performance of correlated-light imaging and that of traditional imaging methods. In this article, we address this issue by exploiting the photon number correlations intrinsic in chaotic light, combined with a cutting-edge ultrafast sensor made of a large array of single-photon avalanche diodes (SPADs). This combination of source and sensor is embedded within a novel single-lens CPI scheme enabling to acquire 10 volumetric images per second. Our results place correlated-photon imaging at a competitive edge and prove its potential in practical applications.

Deconvolution by finite-size-source effects of x-ray phase-contrast images.

PURPOSE: In the hard x-ray region, the cross sections for the phase shift of low-Z elements are about 1000 times larger than the absorption ones. As a consequence, phase contrast is detectable even when absorption contrast is minimal or absent. Therefore, phase-contrast imaging could become a valid alternative to absorption contrast without delivering high dose to tissue/human body parts. METHODS: To enhance the quality of phase-contrast images without increasing the dose, a possible approach could be the partial deconvolution of the finite source size effects by experimental phase-contrast images. The deconvolution procedure, the authors propose, employs the acquisition of two images on a suitable well-known test sample, one in contact and the other in phase-contrast conditions. Both acquired images are used along with a simulated phase-contrast image (obtained from the test sample in ideal conditions of pointlike source illumination) to correctly retrieve the experimental source distribution function. This information allows a generic experimental phase-contrast image, acquired in the same conditions, to be partially deconvolved by finite source size effects. RESULTS: The performed experimental tests indicate that deconvolved images are equivalent to those which would be obtained with a source 40% smaller than the actual size. In turn, this finding is equivalent to an increase of the "effective" lateral spatial coherence length. The corresponding quality improvement of the phase-contrast imaging is directly deducible by the presence of many Fresnel fringes, much better visible with respect to the original experimental phase-contrast images. CONCLUSIONS: The use of a test standard sample, always possible in every experimental setup, to partially deconvolve the finite-size-source blurring effects shows that higher quality phase-contrast images could be readily available, making easier diagnoses and tissue/sample analyses. The method could give, in the future, the possibility to further lower the delivered dose to patients, organs, and tissues when compact room-sized and brilliant microfocus x-ray sources will be available for clinical applications in hospitals.

Multilayer Diffraction Reveals That Colloidal Superlattices Approach the Structural Perfection of Single Crystals.

Colloidal superlattices are fascinating materials made of ordered nanocrystals, yet they are rarely called "atomically precise". That is unsurprising, given how challenging it is to quantify the degree of structural order in these materials. However, once that order crosses a certain threshold, the constructive interference of X-rays diffracted by the nanocrystals dominates the diffraction pattern, offering a wealth of structural information. By treating nanocrystals as scattering sources forming a self-probing interferometer, we developed a multilayer diffraction method that enabled the accurate determination of the nanocrystal size, interparticle spacing, and their fluctuations for samples of self-assembled CsPbBr3 and PbS nanomaterials. The multilayer diffraction method requires only a laboratory-grade diffractometer and an open-source fitting algorithm for data analysis. The average nanocrystal displacement of 0.33 to 1.43 Å in the studied superlattices provides a figure of merit for their structural perfection and approaches the atomic displacement parameters found in traditional crystals.

Combined mixed approach algorithm for in-line phase-contrast x-ray imaging.

PURPOSE: In the past decade, phase-contrast imaging (PCI) has been applied to study different kinds of tissues and human body parts, with an increased improvement of the image quality with respect to simple absorption radiography. A technique closely related to PCI is phase-retrieval imaging (PRI). Indeed, PCI is an imaging modality thought to enhance the total contrast of the images through the phase shift introduced by the object (human body part); PRI is a mathematical technique to extract the quantitative phase-shift map from PCI. A new phase-retrieval algorithm for the in-line phase-contrast x-ray imaging is here proposed. METHODS: The proposed algorithm is based on a mixed transfer-function and transport-of-intensity approach (MA) and it requires, at most, an initial approximate estimate of the average phase shift introduced by the object as prior knowledge. The accuracy in the initial estimate determines the convergence speed of the algorithm. The proposed algorithm retrieves both the object phase and its complex conjugate in a combined MA (CMA). RESULTS: Although slightly less computationally effective with respect to other mixed-approach algorithms, as two phases have to be retrieved, the results obtained by the CMA on simulated data have shown that the obtained reconstructed phase maps are characterized by particularly low normalized mean square errors. The authors have also tested the CMA on noisy experimental phase-contrast data obtained by a suitable weakly absorbing sample consisting of a grid of submillimetric nylon fibers as well as on a strongly absorbing object made of a 0.03 mm thick lead x-ray resolution star pattern. The CMA has shown a good efficiency in recovering phase information, also in presence of noisy data, characterized by peak-to-peak signal-to-noise ratios down to a few dBs, showing the possibility to enhance with phase radiography the signal-to-noise ratio for features in the submillimetric scale with respect to the attenuation-based imaging. CONCLUSIONS: It has been shown that phase-retrieved radiographies can be used both to have quantitative phase information about soft tissues, complementary to the attenuation information, and to enhance the visibility of details inside soft tissues, with higher efficiency with respect to phase radiography.

Table-top combined scanning X-ray small angle scattering and transmission microscopies of lipid vesicles dispersed in free-standing gel.

A mm thick free-standing gel containing lipid vesicles made of 2-oleoyl-1-palmitoyl-sn-glycero-3-phosphocholine (POPC) was studied by scanning Small Angle X-ray Scattering (SAXS) and X-ray Transmission (XT) microscopies. Raster scanning relatively large volumes, besides reducing the risk of radiation damage, allows signal integration, improving the signal-to-noise ratio (SNR), as well as high statistical significance of the dataset. The persistence of lipid vesicles in gel was demonstrated, while mapping their spatial distribution and concentration gradients. Information about lipid aggregation and packing, as well as about gel density gradients, was obtained. A posteriori confirmation of lipid presence in well-defined sample areas was obtained by studying the dried sample, featuring clear Bragg peaks from stacked bilayers. The comparison between wet and dry samples allowed it to be proved that lipids do not significantly migrate within the gel even upon drying, whereas bilayer curvature is lost by removing water, resulting in lipids packed in ordered lamellae. Suitable algorithms were successfully employed for enhancing transmission microscopy sensitivity to low absorbing objects, and allowing full SAXS intensity normalization as a general approach. In particular, data reduction includes normalization of the SAXS intensity against the local sample thickness derived from absorption contrast maps. The proposed study was demonstrated by a room-sized instrumentation, although equipped with a high brilliance X-ray micro-source, and is expected to be applicable to a wide variety of organic, inorganic, and multicomponent systems, including biomaterials. The employed routines for data reduction and microscopy, including Gaussian filter for contrast enhancement of low absorbing objects and a region growing segmentation algorithm to exclude no-sample regions, have been implemented and made freely available through the updated in-house developed software SUNBIM.

X-ray ptychographic mode of self-assembled CdSe/CdS octapod-shaped nanocrystals in thick polymers.

This work describes the application of X-ray ptychography for the inspection of complex assemblies of highly anisotropic nanocrystals embedded in a thick polymer matrix. More specifically, this case deals with CdSe/CdS octapods, with pod length L = 39 ± 2 nm and pod diameter D = 12 ± 2 nm, dispersed in free-standing thick films (24 ± 4 µm) of polymethyl methacrylate and polystyrene, with different molecular weights. Ptychography is the only imaging method available to date that can be used to study architectures made by these types of nanocrystals in thick polymeric films, as any other alternative direct method, such as scanning/transmission electron microscopy, can be definitively ruled out as a result of the large thickness of the free-standing films. The electron density maps of the investigated samples are reconstructed by combining iterative difference map algorithms and a maximum likelihood optimization algorithm. In addition, post image processing techniques are applied to both reduce noise and provide a better visualization of the material morphological details. Through this process, at a final resolution of 27 nm, the reconstructed maps allow us to visualize the intricate network of octapods inside the polymeric matrices.

Coherent Diffraction Imaging in Transmission Electron Microscopy for Atomic Resolution Quantitative Studies of the Matter.

The paper focuses on the development of electron coherent diffraction imaging in transmission electron microscopy, made in the, approximately, last ten years in our collaborative research group, to study the properties of materials at atomic resolution, overcoming the limitations due to the aberrations of the electron lenses and obtaining atomic resolution images, in which the distribution of the maxima is directly related to the specimen atomic potentials projected onto the microscope image detector. Here, it is shown how augmented coherent diffraction imaging makes it possible to achieve quantitative atomic resolution maps of the specimen atomic species, even in the presence of low atomic number atoms within a crystal matrix containing heavy atoms. This aim is achieved by: (i) tailoring the experimental set-up, (ii) improving the experimental data by properly treating parasitic diffused intensities to maximize the measure of the significant information, (iii) developing efficient methods to merge the information acquired in both direct and reciprocal spaces, (iv) treating the dynamical diffused intensities to accurately measure the specimen projected potentials, (v) improving the phase retrieval algorithms to better explore the space of solutions. Finally, some of the future perspectives of coherent diffraction imaging in a transmission electron microscope are given.

Relationship between nano/micro structure and physical properties of TiO2-sodium caseinate composite films.

Films obtained by casting, starting from conventional emulsions (CE), nanoemulsions (NE) or their gels, which led to different structures, with the aim of explore the relationship between structure and physical properties, were prepared. Sodium caseinate was used as the matrix, glycerol as plasticizer, glucono-delta-lactone as acidulant to form the gels, and TiO2 nanoparticles as reinforcement to improve physical behavior. Structural characterization was performed by SAXS and WAXS (Small and Wide Angle X-ray Scattering, respectively), combined with confocal and scanning electron microscopy. The results demonstrate that the incorporation of the lipid phase does not notably modify the mechanical properties of the films compared to solution films. Films from NE were more stable against oil release than those from CE. Incorporation of TiO2 improved mechanical properties as measured by dynamical mechanical analysis (DMA) and uniaxial tensile tests. TiO2 macroscopic spatial distribution homogeneity and the nanostructure character of NE films were confirmed by mapping the q-dependent scattering intensity in scanning SAXS experiments. SAXS microscopies indicated a higher intrinsic homogeneity of NE films compared to CE films, independently of the TiO2 load. NE-films containing structures with smaller and more homogeneously distributed building blocks showed greater potential for food applications than the films prepared from sodium caseinate solutions, which are the best known films.

Facing the phase problem in Coherent Diffractive Imaging via Memetic Algorithms.

Coherent Diffractive Imaging is a lensless technique that allows imaging of matter at a spatial resolution not limited by lens aberrations. This technique exploits the measured diffraction pattern of a coherent beam scattered by periodic and non-periodic objects to retrieve spatial information. The diffracted intensity, for weak-scattering objects, is proportional to the modulus of the Fourier Transform of the object scattering function. Any phase information, needed to retrieve its scattering function, has to be retrieved by means of suitable algorithms. Here we present a new approach, based on a memetic algorithm, i.e. a hybrid genetic algorithm, to face the phase problem, which exploits the synergy of deterministic and stochastic optimization methods. The new approach has been tested on simulated data and applied to the phasing of transmission electron microscopy coherent electron diffraction data of a SrTiO3 sample. We have been able to quantitatively retrieve the projected atomic potential, and also image the oxygen columns, which are not directly visible in the relevant high-resolution transmission electron microscopy images. Our approach proves to be a new powerful tool for the study of matter at atomic resolution and opens new perspectives in those applications in which effective phase retrieval is necessary.