Correcting directional dark field x-ray imaging artefacts using position dependent image deblurring and attenuation removal.

In recent years, a novel x-ray imaging modality has emerged that reveals unresolved sample microstructure via a "dark-field image", which provides complementary information to conventional "bright-field" images, such as attenuation and phase-contrast modalities. This x-ray dark-field signal is produced by unresolved microstructures scattering the x-ray beam resulting in localised image blur. Dark-field retrieval techniques extract this blur to reconstruct a dark-field image. Unfortunately, the presence of non-dark-field blur such as source-size blur or the detector point-spread-function can affect the dark-field retrieval as they also blur the experimental image. In addition, dark-field images can be degraded by the artefacts induced by large intensity gradients from attenuation and propagation-based phase contrast, particularly around sample edges. By measuring any non-dark-field blurring across the image plane and removing it from experimental images, as well as removing attenuation and propagation-based phase contrast, we show that a directional dark-field image can be retrieved with fewer artefacts and more consistent quantitative measures. We present the details of these corrections and provide "before and after" directional dark-field images of samples imaged at a synchrotron source. This paper utilises single-grid directional dark-field imaging, but these corrections have the potential to be broadly applied to other x-ray imaging techniques.

Signal-to-noise and spatial resolution in in-line imaging. 1. Basic theory, numerical simulations and planar experimental images.

Signal-to-noise ratio and spatial resolution are quantitatively analysed in the context of in-line (propagation based) X-ray phase-contrast imaging. It is known that free-space propagation of a coherent X-ray beam from the imaged object to the detector plane, followed by phase retrieval in accordance with Paganin's method, can increase the signal-to-noise in the resultant images without deteriorating the spatial resolution. This results in violation of the noise-resolution uncertainty principle and demonstrates `unreasonable' effectiveness of the method. On the other hand, when the process of free-space propagation is performed in software, using the detected intensity distribution in the object plane, it cannot reproduce the same effectiveness, due to the amplification of photon shot noise. Here, it is shown that the performance of Paganin's method is determined by just two dimensionless parameters: the Fresnel number and the ratio of the real decrement to the imaginary part of the refractive index of the imaged object. The relevant theoretical analysis is performed first, followed by computer simulations and then by a brief test using experimental images collected at a synchrotron beamline. More extensive experimental tests will be presented in the second part of this paper.

X-ray phase and dark-field computed tomography without optical elements.

X-ray diffusive dark-field imaging, which allows spatially unresolved microstructure to be mapped across a sample, is an increasingly popular tool in an array of settings. Here, we present a new algorithm for phase and dark-field computed tomography based on the x-ray Fokker-Planck equation. Needing only a coherent x-ray source, sample, and detector, our propagation-based algorithm can map the sample density and dark-field/diffusion properties of the sample in 3D. Importantly, incorporating dark-field information in the density reconstruction process enables a higher spatial resolution reconstruction than possible with previous propagation-based approaches. Two sample exposures at each projection angle are sufficient for the successful reconstruction of both the sample density and dark-field Fokker-Planck diffusion coefficients. We anticipate that the proposed algorithm may be of benefit in biomedical imaging and industrial settings.

Mask design, fabrication, and experimental ghost imaging applications for patterned X-ray illumination.

A set of non-configurable transversely-displaced masks has been designed and fabricated to generate high-quality X-ray illumination patterns for use in imaging techniques such as ghost imaging (GI), ghost projection, and speckle tracking. The designs include a range of random binary and orthogonal patterns, fabricated through a combination of photolithography and gold electroplating techniques. We experimentally demonstrated that a single wafer can be used as an illumination mask for GI, employing individual illumination patterns and also a mixture of patterns, using a laboratory X-ray source. The quality of the reconstructed X-ray ghost images has been characterized and evaluated through a range of metrics.

On the quantification of sample microstructure using single-exposure x-ray dark-field imaging via a single-grid setup.

The size of the smallest detectable sample feature in an x-ray imaging system is usually restricted by the spatial resolution of the system. This limitation can now be overcome using the diffusive dark-field signal, which is generated by unresolved phase effects or the ultra-small-angle x-ray scattering from unresolved sample microstructures. A quantitative measure of this dark-field signal can be useful in revealing the microstructure size or material for medical diagnosis, security screening and materials science. Recently, we derived a new method to quantify the diffusive dark-field signal in terms of a scattering angle using a single-exposure grid-based approach. In this manuscript, we look at the problem of quantifying the sample microstructure size from this single-exposure dark-field signal. We do this by quantifying the diffusive dark-field signal produced by 5 different sizes of polystyrene microspheres, ranging from 1.0 to 10.8 µm, to investigate how the strength of the extracted dark-field signal changes with the sample microstructure size, [Formula: see text]. We also explore the feasibility of performing single-exposure dark-field imaging with a simple equation for the optimal propagation distance, given microstructure with a specific size and thickness, and show consistency between this model and experimental data. Our theoretical model predicts that the dark-field scattering angle is inversely proportional to [Formula: see text], which is also consistent with our experimental data.

Multimodal intrinsic speckle-tracking (MIST) to extract images of rapidly-varying diffuse X-ray dark-field.

Speckle-based phase-contrast X-ray imaging (SB-PCXI) can reconstruct high-resolution images of weakly-attenuating materials that would otherwise be indistinguishable in conventional attenuation-based X-ray imaging. The experimental setup of SB-PCXI requires only a sufficiently coherent X-ray source and spatially random mask, positioned between the source and detector. The technique can extract sample information at length scales smaller than the imaging system's spatial resolution; this enables multimodal signal reconstruction. "Multimodal Intrinsic Speckle-Tracking" (MIST) is a rapid and deterministic formalism derived from the paraxial-optics form of the Fokker-Planck equation. MIST simultaneously extracts attenuation, refraction, and small-angle scattering (diffusive dark-field) signals from a sample and is more computationally efficient compared to alternative speckle-tracking approaches. Hitherto, variants of MIST have assumed the diffusive dark-field signal to be spatially slowly varying. Although successful, these approaches have been unable to well-describe unresolved sample microstructure whose statistical form is not spatially slowly varying. Here, we extend the MIST formalism such that this restriction is removed, in terms of a sample's rotationally-isotropic diffusive dark-field signal. We reconstruct multimodal signals of two samples, each with distinct X-ray attenuation and scattering properties. The reconstructed diffusive dark-field signals have superior image quality-as measured by the naturalness image quality evaluator, signal-to-noise ratio, and azimuthally averaged power-spectrum-compared to our previous approaches which assume the diffusive dark-field to be a slowly varying function of transverse position. Our generalisation may assist increased adoption of SB-PCXI in applications such as engineering and biomedical disciplines, forestry, and palaeontology, and is anticipated to aid the development of speckle-based diffusive dark-field tensor tomography.

X-Ray Dark-Field and Phase Retrieval Without Optics, via the Fokker-Planck Equation.

Emerging methods of x-ray imaging that capture phase and dark-field effects are equipping medicine with complementary sensitivity to conventional radiography. These methods are being applied over a wide range of scales, from virtual histology to clinical chest imaging, and typically require the introduction of optics such as gratings. Here, we consider extracting x-ray phase and dark-field signals from bright-field images collected using nothing more than a coherent x-ray source and a detector. Our approach is based on the Fokker-Planck equation for paraxial imaging, which is the diffusive generalization of the transport-of-intensity equation. Specifically, we utilize the Fokker-Planck equation in the context of propagation-based phase-contrast imaging, where we show that two intensity images are sufficient for successful retrieval of both the projected thickness and the dark-field signal associated with the sample. We show the results of our algorithm using both a simulated dataset and an experimental dataset. These demonstrate that the x-ray dark-field signal can be extracted from propagation-based images, and that sample thickness can be retrieved with better spatial resolution when dark-field effects are taken into account. We anticipate the proposed algorithm will be of benefit in biomedical imaging, industrial settings, and other non-invasive imaging applications.

Shot-to-shot two-dimensional photon intensity diagnostics within megahertz pulse-trains at the European XFEL.

Characterizing the properties of X-ray free-electron laser (XFEL) sources is a critical step for optimization of performance and experiment planning. The recent availability of MHz XFELs has opened up a range of new opportunities for novel experiments but also highlighted the need for systematic measurements of the source properties. Here, MHz-enabled beam imaging diagnostics developed for the SPB/SFX instrument at the European XFEL are exploited to measure the shot-to-shot intensity statistics of X-ray pulses. The ability to record pulse-integrated two-dimensional transverse intensity measurements at multiple planes along an XFEL beamline at MHz rates yields an improved understanding of the shot-to-shot photon beam intensity variations. These variations can play a critical role, for example, in determining the outcome of single-particle imaging experiments and other experiments that are sensitive to the transverse profile of the incident beam. It is observed that shot-to-shot variations in the statistical properties of a recorded ensemble of radiant intensity distributions are sensitive to changes in electron beam current density. These changes typically occur during pulse-distribution to the instrument and are currently not accounted for by the existing suite of imaging diagnostics. Modulations of the electron beam orbit in the accelerator are observed to induce a time-dependence in the statistics of individual pulses - this is demonstrated by applying radio-frequency trajectory tilts to electron bunch-trains delivered to the instrument. We discuss how these modifications of the beam trajectory might be used to modify the statistical properties of the source and potential future applications.

A Method for High-Resolution Three-Dimensional Reconstruction with Ewald Sphere Curvature Correction from Transmission Electron Images.

A method for three-dimensional reconstruction of objects from defocused images collected at multiple illumination directions in high-resolution transmission electron microscopy is presented. The method effectively corrects for the Ewald sphere curvature by taking into account the in-particle propagation of the electron beam. Numerical simulations demonstrate that the proposed method is capable of accurately reconstructing biological molecules or nanoparticles from high-resolution defocused images under conditions achievable in single-particle electron cryo-microscopy or electron tomography with realistic radiation doses, non-trivial aberrations, multiple scattering, and other experimentally relevant factors. The physics of the method is based on the well-known Diffraction Tomography formalism, but with the phase-retrieval step modified to include a conjugation of the phase (i.e., multiplication of the phase by a negative constant). At each illumination direction, numerically backpropagating the beam with the conjugated phase produces maximum contrast at the location of individual atoms in the molecule or nanoparticle. The resultant algorithm, Conjugated Holographic Reconstruction, can potentially be incorporated into established software tools for single-particle analysis, such as, for example, RELION or FREALIGN, in place of the conventional contrast transfer function correction procedure, in order to account for the Ewald sphere curvature and improve the spatial resolution of the three-dimensional reconstruction.

Dark-field tomography of an attenuating object using intrinsic x-ray speckle tracking.

Purpose: We investigate how an intrinsic speckle tracking approach to speckle-based x-ray imaging is used to extract an object's effective dark-field (DF) signal, which is capable of providing object information in three dimensions. Approach: The effective DF signal was extracted using a Fokker-Planck type formalism, which models the deformations of illuminating reference beam speckles due to both coherent and diffusive scatter from the sample. Here, we assumed that (a) small-angle scattering fans at the exit surface of the sample are rotationally symmetric and (b) the object has both attenuating and refractive properties. The associated inverse problem of extracting the effective DF signal was numerically stabilized using a "weighted determinants" approach. Results: Effective DF projection images, as well as the DF tomographic reconstructions of the wood sample, are presented. DF tomography was performed using a filtered back projection reconstruction algorithm. The DF tomographic reconstructions of the wood sample provided complementary, and otherwise inaccessible, information to augment the phase contrast reconstructions, which were also computed. Conclusions: An intrinsic speckle tracking approach to speckle-based imaging can tomographically reconstruct an object's DF signal at a low sample exposure and with a simple experimental setup. The obtained DF reconstructions have an image quality comparable to alternative x-ray DF techniques.

Unsteady dynamics of a classical particle-wave entity.

A droplet bouncing on the surface of a vertically vibrating liquid bath can walk horizontally, guided by the waves it generates on each impact. This results in a self-propelled classical particle-wave entity. By using a one-dimensional theoretical pilot-wave model with a generalized wave form, we investigate the dynamics of this particle-wave entity. We employ different spatial wave forms to understand the role played by both wave oscillations and spatial wave decay in the walking dynamics. We observe steady walking motion as well as unsteady motions such as oscillating walking, self-trapped oscillations, and irregular walking. We explore the dynamical and statistical aspects of irregular walking and show an equivalence between the droplet dynamics and the Lorenz system, as well as making connections with the Langevin equation and deterministic diffusion.

Comparison of X-ray speckle-based imaging deflection retrieval algorithms for the optimization of radiation dose.

X-ray phase contrast imaging can provide improved or complementary information to traditional attenuation-based X-ray imaging, making the field a vast and rapidly evolving research subject. X-ray speckle-based imaging (SBI) is one phase-contrast imaging approach that has shown significant potential in providing both high sensitivity and high resolution while using a very simple experimental setup. With the aim of transferring such phase-contrast-based imaging techniques from synchrotron to laboratory X-ray sources, the issue of the deposited radiation dose still remains to be addressed. In this work, we experimentally and quantitatively compare the results from three different SBI phase retrieval algorithms using both phantoms and biological samples in order to infer the optimal configuration. The results obtained using a synchrotron beam suggest that the technique based on optical flow conservation achieves the most accurate retrieval from the lowest number of sample exposures. This constitutes an important step toward the possibility of transferring SBI into the clinic.

Recovery of undamaged electron-density maps in the presence of damage-induced partial coherence in single-particle imaging.

Resolving the electronic structure of single biological molecules in their native state was among the primary motivations behind X-ray free-electron lasers. The ultra-short pulses they produce can outrun the atomic motion induced by radiation damage, but the electronic structure of the sample is still significantly modified from its original state. This paper explores the decoherence of the scattered signal induced by temporal evolution of the electronic structure in the sample molecule. It is shown that the undamaged electron density of a single-molecule sample can often be retrieved using only the two most occupied modes from the coherent mode decomposition of the partially coherent diffraction fluence.

Spectral x-ray imaging: Conditions under which propagation-based phase-contrast is beneficial.

Energy-resolved attenuation data in spectral x-ray imaging enables material decomposition, in which the different materials inside an object can be identified and separated virtually. Material decomposition has the drawback of increased noise in the resulting material images relative to the measured images. Recently, spectral x-ray imaging was combined with propagation-based x-ray phase-contrast imaging, an x-ray technique that has the potential to greatly reduce image noise by utilizing wave-optical effects. The net combined effects on image noise of performing spectral material decomposition with phase-contrast are not yet well understood, and we provide a detailed theoretical investigation of this topic here. In particular, we investigate how the addition of phase-contrast in spectral imaging affects material decomposition compared to using conventional spectral attenuation data. We show how the underlying equations can be rearranged into parts that resemble low- and high-pass filters on the input images, from which we are able to identify different energy-dependent cases where phase-contrast is or is not advantageous. Our results suggest that the benefits of phase-contrast in the context of material decomposition are primarily restricted to x-ray energies under a certain threshold, where that threshold depends on the given material combination, and sits in a region where photoelectric absorption dominates x-ray attenuation. Additionally, we show that decomposition of the electron density using an image basis spanned by functions of the Alvarez-Macovski model benefits from phase-contrast, regardless of the x-ray energies. All our findings are based purely on theoretical considerations, and can, therefore, be used to determine the feasibility and utility of propagation-based phase-contrast in spectral x-ray imaging ahead of any data collection.

Noise-resolution uncertainty principle in classical and quantum systems.

We show that the width of an arbitrary function and the width of the distribution of its values cannot be made arbitrarily small simultaneously. In the case of ergodic stochastic processes, an ensuing uncertainty relationship is then demonstrated for the product of correlation length and variance. A closely related uncertainty principle is also established for the average degree of fourth-order coherence and the spatial width of modes of bosonic quantum fields. However, it is shown that, in the case of stochastic and quantum observables, certain non-classical states with sub-Poissonian statistics, such as for example photon number squeezed states in quantum optics, can overcome the "classical" noise-resolution uncertainty limit. This uncertainty relationship, which is fundamentally different from the Heisenberg and related uncertainty principles, can define an upper limit for the information capacity of communication and imaging systems. It is expected to be useful in a variety of problems in classical and quantum optics and imaging.

Hybrid refractive-diffractive axicons for Bessel-beam multiplexing and resolution improvement.

Optical elements rely on refraction, diffraction, or reflection for light manipulation. Fusing diffractive and refractive functions in a single element provides an extra layer of control over the wave propagation, allowing complex beam shaping through self-aligned, monolithic and miniaturized optics. Using gray-scale lithography with high-current focused Xe ion-beams, we realized hybrid refractive-diffractive micro-axicons that feature diffractive gratings engraved on their conical surfaces. Furthermore, we fabricated these devices in lithium niobate, which is a challenging piezo/optoelectronic material for processing with an as-yet unexploited potential in optical applications. The curvilinear surfaces of fabricated micro-axicons with a 230-µm diameter were engraved with diffraction linear and circular gratings of various depths (<400 nm), and the optical performance of these components was characterized, showing excellent agreement with theoretical expectations. The fusing of diffractive elements with carrier refractive surfaces introduces additional or enhanced device functionalities, such as beam multiplexing and resolution improvement. The potential applications of such monolithic and miniaturized hybrid micro-optical components include beamshaping for fluorescence microscopy.

Photon-counting, energy-resolving and super-resolution phase contrast X-ray imaging using an integrating detector.

This work demonstrates the use of a scientific-CMOS (sCMOS) energy-integrating detector as a photon-counting detector, thereby eliminating dark current and read-out noise issues, that simultaneously provides both energy resolution and sub-pixel spatial resolution for X-ray imaging. These capabilities are obtained by analyzing visible light photon clouds that result when X-ray photons produce fluorescence from a scintillator in front of the visible light sensor. Using low-fluence monochromatic X-ray projections to avoid overlapping photon clouds, the centroid of individual X-ray photon interactions was identified. This enabled a tripling of the spatial resolution of the detector to 6.71 ± 0.04 µm. By calculating the total charge deposited by this interaction, an energy resolution of 61.2 ± 0.1% at 17 keV was obtained. When combined with propagation-based phase contrast imaging and phase retrieval, a signal-to-noise ratio of up to 15 ± 3 was achieved for an X-ray fluence of less than 3 photons/mm2.

Model-Based Iterative Reconstruction for Propagation-Based Phase-Contrast X-Ray CT including Models for the Source and the Detector.

Propagation-based phase-contrast X-ray computed tomography is a valuable tool for high-resolution visualization of biological samples, giving distinct improvements in terms of contrast and dose requirements compared to conventional attenuation-based computed tomography. Due to its ease of implementation and advances in laboratory X-ray sources, this imaging technique is increasingly being transferred from synchrotron facilities to laboratory environments. This however poses additional challenges, such as the limited spatial coherence and flux of laboratory sources, resulting in worse resolution and higher noise levels. Here we extend a previously developed iterative reconstruction algorithm for this imaging technique to include models for the reduced spatial coherence and the signal spreading of efficient scintillator-based detectors directly into the physical forward model. Furthermore, we employ a noise model which accounts for the full covariance statistics of the image formation process. In addition, we extend the model describing the interference effects such that it now matches the formalism of the widely-used single-material phase-retrieval algorithm, which is based on the sample-homogeneity assumption. We perform a simulation study as well as an experimental study at a laboratory inverse Compton source and compare our approach to the conventional analytical approaches. We find that the modeling of the source and the detector inside the physical forward model can tremendously improve the resolution at matched noise levels and that the modeling of the covariance statistics reduces overshoots (i.e. incorrect increase / decrease in sample properties) at the sample edges significantly.

Applying the Fokker-Planck equation to grating-based x-ray phase and dark-field imaging.

X-ray imaging has conventionally relied upon attenuation to provide contrast. In recent years, two complementary modalities have been added; (a) phase contrast, which can capture low-density samples that are difficult to see using attenuation, and (b) dark-field x-ray imaging, which reveals the presence of sub-pixel sample structures. These three modalities can be accessed using a crystal analyser, a grating interferometer or by looking at a directly-resolved grid, grating or speckle pattern. Grating and grid-based methods extract a differential phase signal by measuring how far a feature in the illumination has been shifted transversely due to the presence of a sample. The dark-field signal is extracted by measuring how the visibility of the structured illumination is decreased, typically due to the presence of sub-pixel structures in a sample. The strength of the dark-field signal may depend on the grating period, the pixel size and the set-up distances, and additional dark-field signal contributions may be seen as a result of strong phase effects or other factors. In this paper we show that the finite-difference form of the Fokker-Planck equation can be applied to describe the drift (phase signal) and diffusion (dark-field signal) of the periodic or structured illumination used in phase contrast x-ray imaging with gratings, in order to better understand any cross-talk between attenuation, phase and dark-field x-ray signals. In future work, this mathematical description could be used as a basis for new approaches to the inverse problem of recovering both phase and dark-field information.