3D and Multimodal X-Ray Microscopy Reveals the Impact of Voids in CIGS Solar Cells.

Small voids in the absorber layer of thin-film solar cells are generally suspected to impair photovoltaic performance. They have been studied on Cu(In,Ga)Se2 cells with conventional laboratory techniques, albeit limited to surface characterization and often affected by sample-preparation artifacts. Here, synchrotron imaging is performed on a fully operational as-deposited solar cell containing a few tens of voids. By measuring operando current and X-ray excited optical luminescence, the local electrical and optical performance in the proximity of the voids are estimated, and via ptychographic tomography, the depth in the absorber of the voids is quantified. Besides, the complex network of material-deficit structures between the absorber and the top electrode is highlighted. Despite certain local impairments, the massive presence of voids in the absorber suggests they only have a limited detrimental impact on performance.

Rapid aberration correction for diffractive X-ray optics by additive manufacturing.

Diffraction-limited hard X-ray optics are key components for high-resolution microscopy, in particular for upcoming synchrotron radiation sources with ultra-low emittance. Diffractive optics like multilayer Laue lenses (MLL) have the potential to reach unprecedented numerical apertures (NA) when used in a crossed geometry of two one-dimensionally focusing lenses. However, minuscule fluctuations in the manufacturing process and technical limitations for high NA X-ray lenses can prevent a diffraction-limited performance. We present a method to overcome these challenges with a tailor-made refractive phase plate. With at-wavelength metrology and a rapid prototyping approach we demonstrate aberration correction for a crossed pair of MLL, improving the Strehl ratio from 0.41(2) to 0.81(4) at a numerical aperture of 3.3 × 10-3. This highly adaptable aberration-correction scheme provides an important tool for diffraction-limited hard X-ray focusing.

Planar refractive lenses made of SiC for high intensity nanofocusing.

We report on the manufacturing and testing of the first nanofocusing refractive lenses made of single-crystal silicon carbide. We introduce the fabrication process based on lithography, followed by deep isotropic etching. The lenses were characterized at the energy of 12 keV at the beamline P06 of the synchrotron radiation source PETRA III. A focal spot of 186 nm×275 nm has been achieved with a lens working distance of 29 mm.

Nanofocusing with aberration-corrected rotationally parabolic refractive X-ray lenses. Corrigendum.

A correction in the paper by Seiboth et al. [(2018). J. Synchrotron Rad. 25, 108-115] is made.

Erratum: Ossig, C., et al. Four-Fold Multi-Modal X-ray Microscopy Measurements of a Cu(In, Ga)Se2 Solar Cell. Materials 2021, 14, 228.

In the original version of our article [...].

Single-pulse phase-contrast imaging at free-electron lasers in the hard X-ray regime.

X-ray free-electron lasers (XFELs) have opened up unprecedented opportunities for time-resolved nano-scale imaging with X-rays. Near-field propagation-based imaging, and in particular near-field holography (NFH) in its high-resolution implementation in cone-beam geometry, can offer full-field views of a specimen's dynamics captured by single XFEL pulses. To exploit this capability, for example in optical-pump/X-ray-probe imaging schemes, the stochastic nature of the self-amplified spontaneous emission pulses, i.e. the dynamics of the beam itself, presents a major challenge. In this work, a concept is presented to address the fluctuating illumination wavefronts by sampling the configuration space of SASE pulses before an actual recording, followed by a principal component analysis. This scheme is implemented at the MID (Materials Imaging and Dynamics) instrument of the European XFEL and time-resolved NFH is performed using aberration-corrected nano-focusing compound refractive lenses. Specifically, the dynamics of a micro-fluidic water-jet, which is commonly used as sample delivery system at XFELs, is imaged. The jet exhibits rich dynamics of droplet formation in the break-up regime. Moreover, pump-probe imaging is demonstrated using an infrared pulsed laser to induce cavitation and explosion of the jet.

Femtosecond electronic structure response to high intensity XFEL pulses probed by iron X-ray emission spectroscopy.

We report the time-resolved femtosecond evolution of the K-shell X-ray emission spectra of iron during high intensity illumination of X-rays in a micron-sized focused hard X-ray free electron laser (XFEL) beam. Detailed pulse length dependent measurements revealed that rapid spectral energy shift and broadening started within the first 10 fs of the X-ray illumination at intensity levels between 1017 and 1018 W cm-2. We attribute these spectral changes to the rapid evolution of high-density photoelectron mediated secondary collisional ionization processes upon the absorption of the incident XFEL radiation. These fast electronic processes, occurring at timescales well within the typical XFEL pulse durations (i.e., tens of fs), set the boundary conditions of the pulse intensity and sample parameters where the widely-accepted 'probe-before-destroy' measurement strategy can be adopted for electronic-structure related XFEL experiments.

Hard X-ray wavefront correction via refractive phase plates made by additive and subtractive fabrication techniques.

Modern subtractive and additive manufacturing techniques present new avenues for X-ray optics with complex shapes and patterns. Refractive phase plates acting as glasses for X-ray optics have been fabricated, and spherical aberration in refractive X-ray lenses made from beryllium has been successfully corrected. A diamond phase plate made by femtosecond laser ablation was found to improve the Strehl ratio of a lens stack with a numerical aperture (NA) of 0.88 × 10-3 at 8.2 keV from 0.1 to 0.7. A polymer phase plate made by additive printing achieved an increase in the Strehl ratio of a lens stack at 35 keV with NA of 0.18 × 10-3 from 0.15 to 0.89, demonstrating diffraction-limited nanofocusing at high X-ray energies.

Refractive hard x-ray vortex phase plates.

In this Letter, we report on the creation of hard x-ray beams carrying orbital angular momentum of topological charge -ℏ and -3ℏ at a photon energy of 8.2 keV via spiral phase plates made out of fused silica by ultrashort-pulsed laser ablation. The phase plates feature a smooth phase ramp with a 0.5 µm nominal step height and a surface roughness of 0.5 µm. The measured vortex beams show submicrometer-sized donut rings and agree well with numerical modeling. Fused silica phase plates are potentially suited to manipulate the electromagnetic field in highly intense x-ray beams at x-ray free-electron laser sources.

Wavefront sensing at X-ray free-electron lasers.

Here a direct comparison is made between various X-ray wavefront sensing methods with application to optics alignment and focus characterization at X-ray free-electron lasers (XFELs). Focus optimization at XFEL beamlines presents unique challenges due to high peak powers as well as beam pointing instability, meaning that techniques capable of single-shot measurement and that probe the wavefront at an out-of-focus location are desirable. The techniques chosen for the comparison include single-phase-grating Talbot interferometry (shearing interferometry), dual-grating Talbot interferometry (moiré deflectometry) and speckle tracking. All three methods were implemented during a single beam time at the Linac Coherent Light Source, at the X-ray Pump Probe beamline, in order to make a direct comparison. Each method was used to characterize the wavefront resulting from a stack of beryllium compound refractive lenses followed by a corrective phase plate. In addition, difference wavefront measurements with and without the phase plate agreed with its design to within λ/20, which enabled a direct quantitative comparison between methods. Finally, a path toward automated alignment at XFEL beamlines using a wavefront sensor to close the loop is presented.

Nanofocusing with aberration-corrected rotationally parabolic refractive X-ray lenses.

Wavefront errors of rotationally parabolic refractive X-ray lenses made of beryllium (Be CRLs) have been recovered for various lens sets and X-ray beam configurations. Due to manufacturing via an embossing process, aberrations of individual lenses within the investigated ensemble are very similar. By deriving a mean single-lens deformation for the ensemble, aberrations of any arbitrary lens stack can be predicted from the ensemble with \bar{\sigma} = 0.034λ. Using these findings the expected focusing performance of current Be CRLs are modeled for relevant X-ray energies and bandwidths and it is shown that a correction of aberrations can be realised without prior lens characterization but simply based on the derived lens deformation. The performance of aberration-corrected Be CRLs is discussed and the applicability of aberration-correction demonstrated over wide X-ray energy ranges.

Focal Spot and Wavefront Sensing of an X-Ray Free Electron laser using Ronchi shearing interferometry.

The Linac Coherent Light Source (LCLS) is an X-ray source of unmatched brilliance, that is advancing many scientific fields at a rapid pace. The highest peak intensities that are routinely produced at LCLS take place at the Coherent X-ray Imaging (CXI) instrument, which can produce spotsize at the order of 100 nm, and such spotsizes and intensities are crucial for experiments ranging from coherent diffractive imaging, non-linear x-ray optics and high field physics, and single molecule imaging. Nevertheless, a full characterisation of this beam has up to now not been performed. In this paper we for the first time characterise this nanofocused beam in both phase and intensity using a Ronchi Shearing Interferometric technique. The method is fast, in-situ, uses a straightforward optimization algoritm, and is insensitive to spatial jitter.

Perfect X-ray focusing via fitting corrective glasses to aberrated optics.

Due to their short wavelength, X-rays can in principle be focused down to a few nanometres and below. At the same time, it is this short wavelength that puts stringent requirements on X-ray optics and their metrology. Both are limited by today's technology. In this work, we present accurate at wavelength measurements of residual aberrations of a refractive X-ray lens using ptychography to manufacture a corrective phase plate. Together with the fitted phase plate the optics shows diffraction-limited performance, generating a nearly Gaussian beam profile with a Strehl ratio above 0.8. This scheme can be applied to any other focusing optics, thus solving the X-ray optical problem at synchrotron radiation sources and X-ray free-electron lasers.

The phase-contrast imaging instrument at the matter in extreme conditions endstation at LCLS.

We describe the phase-contrast imaging instrument at the Matter in Extreme Conditions (MEC) endstation of the Linac Coherent Light Source. The instrument can image phenomena with a spatial resolution of a few hundreds of nanometers and at the same time reveal the atomic structure through X-ray diffraction, with a temporal resolution better than 100 fs. It was specifically designed for studies relevant to high-energy-density science and can monitor, e.g., shock fronts, phase transitions, or void collapses. This versatile instrument was commissioned last year and is now available to the MEC user community.

Imaging Shock Waves in Diamond with Both High Temporal and Spatial Resolution at an XFEL.

The advent of hard x-ray free-electron lasers (XFELs) has opened up a variety of scientific opportunities in areas as diverse as atomic physics, plasma physics, nonlinear optics in the x-ray range, and protein crystallography. In this article, we access a new field of science by measuring quantitatively the local bulk properties and dynamics of matter under extreme conditions, in this case by using the short XFEL pulse to image an elastic compression wave in diamond. The elastic wave was initiated by an intense optical laser pulse and was imaged at different delay times after the optical pump pulse using magnified x-ray phase-contrast imaging. The temporal evolution of the shock wave can be monitored, yielding detailed information on shock dynamics, such as the shock velocity, the shock front width, and the local compression of the material. The method provides a quantitative perspective on the state of matter in extreme conditions.

Fast Strain Mapping of Nanowire Light-Emitting Diodes Using Nanofocused X-ray Beams.

X-ray nanobeams are unique nondestructive probes that allow direct measurements of the nanoscale strain distribution and composition inside the micrometer thick layered structures that are found in most electronic device architectures. However, the method is usually extremely time-consuming, and as a result, data sets are often constrained to a few or even single objects. Here we demonstrate that by special design of a nanofocused X-ray beam diffraction experiment we can (in a single 2D scan with no sample rotation) measure the individual strain and composition profiles of many structures in an array of upright standing nanowires. We make use of the observation that in the generic nanowire device configuration, which is found in high-speed transistors, solar cells, and light-emitting diodes, each wire exhibits very small degrees of random tilts and twists toward the substrate. Although the tilt and twist are very small, they give a new contrast mechanism between different wires. In the present case, we image complex nanowires for nanoLED fabrication and compare to theoretical simulations, demonstrating that this fast method is suitable for real nanostructured devices.

Focus characterization at an X-ray free-electron laser by coherent scattering and speckle analysis.

X-ray focus optimization and characterization based on coherent scattering and quantitative speckle size measurements was demonstrated at the Linac Coherent Light Source. Its performance as a single-pulse free-electron laser beam diagnostic was tested for two typical focusing configurations. The results derived from the speckle size/shape analysis show the effectiveness of this technique in finding the focus' location, size and shape. In addition, its single-pulse compatibility enables users to capture pulse-to-pulse fluctuations in focus properties compared with other techniques that require scanning and averaging.

Ronchi test for characterization of X-ray nanofocusing optics and beamlines.

A Ronchi interferometer for hard X-rays is reported in order to characterize the performance of the nanofocusing optics as well as the beamline stability. Characteristic interference fringes yield qualitative data on present aberrations in the optics. Moreover, the visibility of the fringes on the detector gives information on the degree of spatial coherence in the beamline. This enables the possibility to detect sources of instabilities in the beamline like vibrations of components or temperature drift. Examples are shown for two different nanofocusing hard X-ray optics: a compound refractive lens and a zone plate.

Damage investigation on tungsten and diamond diffractive optics at a hard x-ray free-electron laser.

Focusing hard x-ray free-electron laser radiation with extremely high fluence sets stringent demands on the x-ray optics. Any material placed in an intense x-ray beam is at risk of being damaged. Therefore, it is crucial to find the damage thresholds for focusing optics. In this paper we report experimental results of exposing tungsten and diamond diffractive optics to a prefocused 8.2 keV free-electron laser beam in order to find damage threshold fluence levels. Tungsten nanostructures were damaged at fluence levels above 500 mJ/cm(2). The damage was of mechanical character, caused by thermal stress variations. Diamond nanostructures were affected at a fluence of 59 000 mJ/cm(2). For fluence levels above this, a significant graphitization process was initiated. Scanning Electron Microscopy (SEM) and µ-Raman analysis were used to analyze exposed nanostructures.

Full spatial characterization of a nanofocused x-ray free-electron laser beam by ptychographic imaging.

The emergence of hard X-ray free electron lasers (XFELs) enables new insights into many fields of science. These new sources provide short, highly intense, and coherent X-ray pulses. In a variety of scientific applications these pulses need to be strongly focused. In this article, we demonstrate focusing of hard X-ray FEL pulses to 125 nm using refractive x-ray optics. For a quantitative analysis of most experiments, the wave field or at least the intensity distribution illuminating the sample is needed. We report on the full characterization of a nanofocused XFEL beam by ptychographic imaging, giving access to the complex wave field in the nanofocus. From these data, we obtain the full caustic of the beam, identify the aberrations of the optic, and determine the wave field for individual pulses. This information is for example crucial for high-resolution imaging, creating matter in extreme conditions, and nonlinear x-ray optics.