Search for Dark Matter Annihilation Signals in the H.E.S.S. Inner Galaxy Survey.

The central region of the Milky Way is one of the foremost locations to look for dark matter (DM) signatures. We report the first results on a search for DM particle annihilation signals using new observations from an unprecedented γ-ray survey of the Galactic Center (GC) region, i.e., the Inner Galaxy Survey, at very high energies (≳100 GeV) performed with the H.E.S.S. array of five ground-based Cherenkov telescopes. No significant γ-ray excess is found in the search region of the 2014-2020 dataset and a profile likelihood ratio analysis is carried out to set exclusion limits on the annihilation cross section ⟨σv⟩. Assuming Einasto and Navarro-Frenk-White (NFW) DM density profiles at the GC, these constraints are the strongest obtained so far in the TeV DM mass range. For the Einasto profile, the constraints reach ⟨σv⟩ values of 3.7×10^{-26} cm^{3} s^{-1} for 1.5 TeV DM mass in the W^{+}W^{-} annihilation channel, and 1.2×10^{-26} cm^{3} s^{-1} for 0.7 TeV DM mass in the τ^{+}τ^{-} annihilation channel. With the H.E.S.S. Inner Galaxy Survey, ground-based γ-ray observations thus probe ⟨σv⟩ values expected from thermal-relic annihilating TeV DM particles.

A Convex Variational Model for Learning Convolutional Image Atoms from Incomplete Data.

A variational model for learning convolutional image atoms from corrupted and/or incomplete data is introduced and analyzed both in function space and numerically. Building on lifting and relaxation strategies, the proposed approach is convex and allows for simultaneous image reconstruction and atom learning in a general, inverse problems context. Further, motivated by an improved numerical performance, also a semi-convex variant is included in the analysis and the experiments of the paper. For both settings, fundamental analytical properties allowing in particular to ensure well-posedness and stability results for inverse problems are proven in a continuous setting. Exploiting convexity, globally optimal solutions are further computed numerically for applications with incomplete, noisy and blurry data and numerical results are shown.

Quantitative region-of-interest tomography using variable field of view.

In X-ray computed tomography, the task of imaging only a local region of interest (ROI) inside a larger sample is very important. However, without a priori information, this ROI cannot be exactly reconstructed using only the image data limited to the ROI. We propose here an approach of region-of-interest tomography, which reconstructs a ROI within an object from projections of different fields of view acquired on a specific angular sampling scheme in the same tomographic experiment. We present a stable procedure that not only yields high-quality images of the ROI but keeps as well the quantitative contrast on the reconstructed images. In addition, we analyze the minimum number of projections required for ROI tomography from the point of view of the band region of the Radon transform, which confirms this number must be estimated based on the size of the entire object and not only on the size of the ROI.

OMNY-A tOMography Nano crYo stage.

For many scientific questions gaining three-dimensional insight into a specimen can provide valuable information. We here present an instrument called "tOMography Nano crYo (OMNY)," dedicated to high resolution 3D scanning x-ray microscopy at cryogenic conditions via hard X-ray ptychography. Ptychography is a lens-less imaging method requiring accurate sample positioning. In OMNY, this in achieved via dedicated laser interferometry and closed-loop position control reaching sub-10 nm positioning accuracy. Cryogenic sample conditions are maintained via conductive cooling. 90 K can be reached when using liquid nitrogen as coolant, and 10 K is possible with liquid helium. A cryogenic sample-change mechanism permits measurements of cryogenically fixed specimens. We compare images obtained with OMNY with older measurements performed using a nitrogen gas cryo-jet of stained, epoxy-embedded retina tissue and of frozen-hydrated Chlamydomonas cells.

OMNY PIN-A versatile sample holder for tomographic measurements at room and cryogenic temperatures.

Nowadays ptychographic tomography in the hard x-ray regime, i.e., at energies above about 2 keV, is a well-established measurement technique. At the Paul Scherrer Institut, currently two instruments are available: one is measuring at room temperature and atmospheric pressure, and the other, the so-called OMNY (tOMography Nano crYo) instrument, is operating at ultra-high vacuum and offering cryogenic sample temperatures down to 10 K. In this manuscript, we present the sample mounts that were developed for these instruments. Aside from excellent mechanical stability and thermal conductivity, they also offer highly reproducible mounting. Various types were developed for different kinds of samples and are presented in detail, including examples of how specimens can be mounted on these holders. We also show the first hard x-ray ptychographic tomography measurements of high-pressure frozen biological samples, in the present case Chlamydomonas cells, the related sample pins and preparation steps. For completeness, we present accessories such as transportation containers for both room temperature and cryogenic samples and a gripper mechanism for automatic sample changing. The sample mounts are not limited to x-ray tomography or hard x-ray energies, and we believe that they can be very useful for other instrumentation projects.

A three-dimensional view of structural changes caused by deactivation of fluid catalytic cracking catalysts.

Since its commercial introduction three-quarters of a century ago, fluid catalytic cracking has been one of the most important conversion processes in the petroleum industry. In this process, porous composites composed of zeolite and clay crack the heavy fractions in crude oil into transportation fuel and petrochemical feedstocks. Yet, over time the catalytic activity of these composite particles decreases. Here, we report on ptychographic tomography, diffraction, and fluorescence tomography, as well as electron microscopy measurements, which elucidate the structural changes that lead to catalyst deactivation. In combination, these measurements reveal zeolite amorphization and distinct structural changes on the particle exterior as the driving forces behind catalyst deactivation. Amorphization of zeolites, in particular, close to the particle exterior, results in a reduction of catalytic capacity. A concretion of the outermost particle layer into a dense amorphous silica-alumina shell further reduces the mass transport to the active sites within the composite.Catalyst deactivation in fluid catalytic cracking processes is unavoidably associated with structural changes. Here, the authors visualize the deactivation of zeolite catalysts by ptychography and other imaging techniques, showing pronounced amorphization of the outer layer of the catalyst particles.

Three-Dimensional Imaging of Biological Tissue by Cryo X-Ray Ptychography.

High-throughput three-dimensional cryogenic imaging of thick biological specimens is valuable for identifying biologically- or pathologically-relevant features of interest, especially for subsequent correlative studies. Unfortunately, high-resolution imaging techniques at cryogenic conditions often require sample reduction through sequential physical milling or sectioning for sufficient penetration to generate each image of the 3-D stack. This study represents the first demonstration of using ptychographic hard X-ray tomography at cryogenic temperatures for imaging thick biological tissue in a chemically-fixed, frozen-hydrated state without heavy metal staining and organic solvents. Applied to mammalian brain, this label-free cryogenic imaging method allows visualization of myelinated axons and sub-cellular features such as age-related pigmented cellular inclusions at a spatial resolution of ~100 nanometers and thicknesses approaching 100 microns. Because our approach does not require dehydration, staining or reduction of the sample, we introduce the possibility for subsequent analysis of the same tissue using orthogonal approaches that are expected to yield direct complementary insight to the biological features of interest.

Clinical Application of Fiber Visualization with LIC Maps Using Multidirectional Anisotropic Glyph Samples (A-Glyph LIC).

Recently, a fiber visualization method for high-angular resolution diffusion-weighted magnetic resonance imaging (MRI) data was proposed using a multiple-kernel line integral convolution (LIC) algorithm and an anisotropic spot pattern. This processing routine leads to high contrast color-coded LIC maps that are capable of visualizing local anisotropy information and regional fiber architecture. In this paper, we evaluate and validate this method by applying it to simulated datasets and to in vivo diffusion MRI data of children and adults with different disease conditions and healthy volunteers. Compared to routine clinical fiber visualization (color-coded fractional anisotropy, FA maps, and fiber tractography), it has the advantage of visualizing complex local fiber architecture in a fully automated way. The results indicate that this method is capable of reliably delineating normal fiber architecture and fibers infiltrated, displaced, or disrupted by lesions and is therefore a promising tool in the clinical context.

Image-Based Personalization of Cardiac Anatomy for Coupled Electromechanical Modeling.

Computational models of cardiac electromechanics (EM) are increasingly being applied to clinical problems, with patient-specific models being generated from high fidelity imaging and used to simulate patient physiology, pathophysiology and response to treatment. Current structured meshes are limited in their ability to fully represent the detailed anatomical data available from clinical images and capture complex and varied anatomy with limited geometric accuracy. In this paper, we review the state of the art in image-based personalization of cardiac anatomy for biophysically detailed, strongly coupled EM modeling, and present our own tools for the automatic building of anatomically and structurally accurate patient-specific models. Our method relies on using high resolution unstructured meshes for discretizing both physics, electrophysiology and mechanics, in combination with efficient, strongly scalable solvers necessary to deal with the computational load imposed by the large number of degrees of freedom of these meshes. These tools permit automated anatomical model generation and strongly coupled EM simulations at an unprecedented level of anatomical and biophysical detail.

Improving organic tandem solar cells based on water-processed nanoparticles by quantitative 3D nanoimaging.

Organic solar cells have great potential for upscaling due to roll-to-roll processing and a low energy payback time, making them an attractive sustainable energy source for the future. Active layers coated with water-dispersible Landfester particles enable greater control of the layer formation and easier access to the printing industry, which has reduced the use of organic solvents since the 1980s. Through ptychographic X-ray computed tomography (PXCT), we image quantitatively a roll-to-roll coated photovoltaic tandem stack consisting of one bulk heterojunction active layer and one Landfester particle active layer. We extract the layered morphology with structural and density information including the porosity present in the various layers and the silver electrode with high resolution in 3D. The Landfester particle layer is found to have an undesired morphology with negatively correlated top- and bottom interfaces, wide thickness distribution and only partial surface coverage causing electric short circuits through the layer. By top coating a polymer material onto the Landfester nanoparticles we eliminate the structural defects of the layer such as porosity and roughness, and achieve the increased performance larger than 1 V expected for a tandem cell. This study highlights that quantitative imaging of weakly scattering stacked layers of organic materials has become feasible by PXCT, and that this information cannot be obtained by other methods. In the present study, this technique specifically reveals the need to improve the coatability and layer formation of Landfester nanoparticles, thus allowing improved solar cells to be produced.

X-ray ptychographic computed tomography at 16 nm isotropic 3D resolution.

X-ray ptychography is a scanning variant of coherent diffractive imaging with the ability to image large fields of view at high resolution. It further allows imaging of non-isolated specimens and can produce quantitative mapping of the electron density distribution in 3D when combined with computed tomography. The method does not require imaging lenses, which makes it dose efficient and suitable to multi-keV X-rays, where efficient photon counting, pixelated detectors are available. Here we present the first highly resolved quantitative X-ray ptychographic tomography of an extended object yielding 16 nm isotropic 3D resolution recorded at 2 Šwavelength. This first-of-its-kind demonstration paves the way for ptychographic X-ray tomography to become a promising method for X-ray imaging of representative sample volumes at unmatched resolution, opening tremendous potential for characterizing samples in materials science and biology by filling the resolution gap between electron microscopy and other X-ray imaging techniques.

An instrument for 3D x-ray nano-imaging.

We present an instrument dedicated to 3D scanning x-ray microscopy, allowing a sample to be precisely scanned through a beam while the angle of x-ray incidence can be changed. The position of the sample is controlled with respect to the beam-defining optics by laser interferometry. The instrument achieves a position stability better than 10 nm standard deviation. The instrument performance is assessed using scanning x-ray diffraction microscopy and we demonstrate a resolution of 18 nm in 2D imaging of a lithographic test pattern while the beam was defined by a pinhole of 3 µm in diameter. In 3D on a test object of copper interconnects of a microprocessor, a resolution of 53 nm is achieved.

Attosecond electron wave-packet interference observed by transient absorption.

We perform attosecond time-resolved transient absorption spectroscopy around the first ionization threshold of helium and observe rapid oscillations of the absorption of the individual harmonics as a function of time delay with respect to a superimposed, moderately strong infrared laser field. The phase relation between the absorption modulation of individual harmonics gives direct evidence for the interference of transiently bound electronic wave packets as the mechanism behind the absorption modulation.

Spatial fingerprint of quantum path interferences in high order harmonic generation.

We have spatially and spectrally resolved the high order harmonic emission from an argon gas target. Under proper phase matching conditions we were able to observe for the first time the spatial fine structure originating from the interference of the two shortest quantum paths in the harmonic beam. The structure can be explained by the intensity-dependent harmonic phase of the contributions from the two paths. The spatially and spectrally resolved measurements are consistent with previous spatially integrated results. Our measurement method represents a new tool to clearly distinguish between different interference effects and to potentially observe higher order trajectories in the future with improved detection sensitivity. Here, we demonstrate additional experimental evidence that the observed interference pattern is only due to quantum-path interferences and cannot be explained by a phase modulation effect. Our experimental results are fully supported by simulations using the strong field approximation and including propagation.

Ionization effects on spectral signatures of quantum-path interference in high-harmonic generation.

The interference between the emission originating from the short and long electron quantum paths is intrinsic to the high harmonic generation process. We investigate the universal properties of these quantum-path interferences in various generation media and discuss how ionization effects influence the observed interference structures. Our comparison of quantum-path interferences observed in xenon, argon, and neon demonstrates that our experimental tools are generally applicable and should also allow investigating more complex systems such as molecules or clusters.

Spectral signature of short attosecond pulse trains.

We report experimental measurements of high-order harmonic spectra generated in Ar using a carrier-envelope-offset (CEO) stabilized 12 fs, 800 nm laser field and a fraction (less than 10%) of its second harmonic. Additional spectral peaks are observed between the harmonic peaks, which are due to interferences between multiple pulses in the train. The position of these peaks varies with the CEO and their number is directly related to the number of pulses in the train. An analytical model, as well as numerical simulations, support our interpretation.

Quantum path interferences in high-order harmonic generation.

We have investigated the intensity dependence of high-order harmonic generation in argon when the two shortest quantum paths contribute to the harmonic emission. For the first time to our knowledge, experimental conditions were found to clearly observe interference between these two quantum paths that are in excellent agreement with theoretical predictions. This result is a first step towards the direct experimental characterization of the full single-atom dipole moment and demonstrates an unprecedented accuracy of quantum path control on an attosecond time scale.

Spatio-temporal characterization of few-cycle pulses obtained by filamentation.

Intense sub-5-fs pulses were generated by filamentation in a noble gas and subsequent chirped-mirror pulse compression. The transversal spatial dependence of the temporal pulse profile was investigated by spatial selection of parts of the output beam. Selecting the central core of the beam is required for obtaining the shortest possible pulses. Higher energy efficiency is only obtained at the expense of pulse contrast since towards the outer parts of the beam the energy is spread into satellite structures leading to a double-pulse profile on the very off-axis part of the beam. Depending on the requirements for a particular application, a trade-off between the pulse duration and the pulse energy has to be done. The energy of the sub-5-fs pulses produced was sufficient for the generation of high order harmonics in Argon. In addition, full simulation is performed in space and time on pulse propagation through filamentation that explains the double-pulse structure observed as part of a conical emission enhanced by the plasma defocusing.

In vivo 3D visualization of normal pyramidal tracts in human subjects using diffusion weighted magnetic resonance imaging and a neuronavigation system.

We describe the potential of anisotropic diffusion weighted imaging to visualize the course of large cerebral fiber tracts. Five healthy volunteers were investigated at a field strength of 1.5 Tesla, employing a spin-echo diffusion weighted sequence with gradient sensitivity in six non-collinear directions to visualize the course of the pyramidal tracts. The pyramidal tracts were segmented and reconstructed for three-dimensional visualization. Reconstruction results together with a fusioned high resolution 3D T1 weighted image data set were available in a customized neuronavigation system. Origination in the primary motor cortex, convergence in the centrum semiovale, the posterior limb of the internal capsule, the cerebral peduncles, the splitting at the level of the pons, and the pyramidal decussation were identified in all subjects. Fiber tract maps might have the prospect of guiding neurosurgical interventions, especially when being linked to a neuronavigation system. Other potential applications include the demonstration of the anatomical substrate of functional connectivity in the human brain.

(E)-1-alkyl-4-

(E)-1-Alkyl-4-[2-(alkylsulfonyl)-1-ethenyl]pyridinium salts were synthesized in two steps. These sulfones were stable at pH 7.3 and underwent a nucleophilic vinylic substitution (S(N)V) with mercaptans, including thiouracile, to give the corresponding 4-(thiovinyl)-pyridinium salts. The X-ray diffraction structure of (E)-1-methyl-4-[2-(ethylsulfanyl)-1-ethenyl]pyridinium iodide indicated conjugation of the sulfur with the pyridinium ring. (Z)-1-Methyl-4-[2-(methylsulfanyl)-1-ethenyl]pyridinium iodide, prepared from the corresponding thioether by reaction with methyl iodide in diethyl ether, underwent isomerization to the E isomer in a first-order reaction in deuterated [D6]DMSO with an activation energy of 14 kcalmol(-1). At pH 7, the (E)-1-methyl-4-[2-(methylsulfonyl)-1-ethenyl]pyridinium iodide (19) reacted specifically with thiols. The reaction of this sulfone with glutathione in a TES buffer at pH 7 was a second-order reaction (k = 4,100 M(-1)s(-1) at 30 degrees C) and gave the corresponding substitution product with an intense long wavelength absorption band (lambdamax=360 nm, epsilon = 27,500 M(-1)cm(-1)). The modification of different enzymes of known structure with 19 showed the high selectivity of this reagent towards thiol groups and its usefulness in the quantitative determination of free thiol groups in proteins.