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.
Single-shot grating-based phase-contrast imaging techniques offer additional contrast modalities based on the refraction and scattering of X-rays in a robust and versatile configuration. The utilization of a single optical element is possible in such methods, allowing the shortening of the acquisition time and increasing flux efficiency. One of the ways to upgrade single-shot imaging techniques is to utilize customized optical components, such as two-dimensional (2D) X-ray gratings. In this contribution, we present the achievements in the development of 2D gratings with UV lithography and gold electroplating. Absorption gratings represented by periodic free-standing gold pillars with lateral structure sizes from 5 µm to 25 µm and heights from 5 µm to 28 µm have shown a high degree of periodicity and defect-free patterns. Grating performance was tested in a radiographic setup using a self-developed quality assessment algorithm based on the intensity distribution histograms. The algorithm allows the final user to estimate the suitability of a specific grating to be used in a particular setup.
Sub-ångström spatial resolution of electron density coupled with sub-femtosecond to few-femtosecond temporal resolution is required to directly observe the dynamics of the electronic structure of a molecule after photoinitiation or some other ultrafast perturbation, such as by soft X-rays. Meeting this challenge, pushing the field of quantum crystallography to attosecond timescales, would bring insights into how the electronic and nuclear degrees of freedom couple, enable the study of quantum coherences involved in molecular dynamics, and ultimately enable these dynamics to be controlled. Here, we propose to reach this realm by employing convergent-beam x-ray crystallography with high-power attosecond pulses from a hard-x-ray free-electron laser. We show that with dispersive optics, such as multilayer Laue lenses of high numerical aperture, it becomes possible to encode time into the resulting diffraction pattern with deep sub-femtosecond precision. Each snapshot diffraction pattern consists of Bragg streaks that can be mapped back to arrival times and positions of X-rays on the face of a crystal. This can span tens of femtoseconds and can be finely sampled as we demonstrate experimentally. The approach brings several other advantages, such as an increase in the number of observable reflections in a snapshot diffraction pattern, all fully integrated, to improve the speed and accuracy of serial crystallography—especially for crystals of small molecules.
In this Letter, we present the application of the inverted Hartmann mask for time-resolved single-shot phase-contrast x-ray imaging. The inverted Hartmann mask is a periodic array of free-standing gold pillars. The array is manufactured by UV lithography and electroplating. Time-resolved measurements are performed for imaging of pulsed laser ablation in liquids using white-beam synchrotron radiation. The inverted Hartmann mask in combination with a single-shot imaging technique provides sufficient differential phase contrast even at very short exposure times. It can be effectively used for phase-contrast x-ray imaging of fast dynamic processes with temporal resolution on the millisecond scale.
The quality of high aspect ratio microstructures fabricated by deep X-ray lithography is highly dependent on the photoresist material used and the process parameters applied. Even with photoresists more suitable to this process, it is common to face defects in the final optical components, such as in case of X-ray gratings. The gratings need to be fabricated with critical dimensions on a sub-micrometer and micrometer scale, with periods of few micrometers and heights of hundreds of micrometers to be used in X-ray imaging techniques such as Talbot–Lau Interferometry. During the fabrication process, these features lead to challenges such as mechanical stability, homogeneity, and defect-free grating patterns. Usually, an epoxy-based negative photoresist is used in X-ray lithography, which needs to account for the shrinkage that takes place during polymer crosslinking in order to avoid defects in the final pattern. Nowadays, photoresist material still lacks certain suitable properties (chemical and mechanical) to fabricate gratings of high quality and with acceptable reproducibility. This work presents the results of TGA, FTIR, and MALDI-TOF analysis made on photoresists commercially available and suitable for X-ray lithography. The photoresists presented different profiles regarding the solvent content and oligomers composition, and in the case of some samples, there were high amounts of non-epoxidized oligomers.
High time resolution in scattering analysis of thin films allows for determination of thermal conductivity by transient pump-probe detection of dissipation of laser-induced heating, TDXTS. We describe an approach that analyses the picosecond-resolved lattice parameter reaction of a gold transducer layer on pulsed laser heating to determine the thermal conductivity of layered structures below the transducer. A detailed modeling of the cooling kinetics by a Laplace-domain approach allows for discerning effects of conductivity and thermal interface resistance as well as basic depth information. The thermal expansion of the clamped gold film can be calibrated to absolute temperature change and effects of plastic deformation are discriminated. The method is demonstrated on two extreme examples of phononic barriers, isotopically modulated silicon multilayers with very small acoustic impedance mismatch and silicon-molybdenum multilayers, which show a high resistivity.