Direct LiF imaging diagnostics on refractive X-ray focusing at the EuXFEL High Energy Density instrument.

The application of fluorescent crystal media in wide-range X-ray detectors provides an opportunity to directly image the spatial distribution of ultra-intense X-ray beams including investigation of the focal spot of free-electron lasers. Here the capabilities of the micro- and nano-focusing X-ray refractive optics available at the High Energy Density instrument of the European XFEL are reported, as measured in situ by means of a LiF fluorescent detector placed into and around the beam caustic. The intensity distribution of the beam focused down to several hundred nanometers was imaged at 9 keV photon energy. A deviation from the parabolic surface in a stack of nanofocusing Be compound refractive lenses (CRLs) was found to affect the resulting intensity distribution within the beam. Comparison of experimental patterns in the far field with patterns calculated for different CRL lens imperfections allowed the overall inhomogeneity in the CRL stack to be estimated. The precise determination of the focal spot size and shape on a sub-micrometer level is essential for a number of high energy density studies requiring either a pin-size backlighting spot or extreme intensities for X-ray heating.

Damage threshold of LiF crystal irradiated by femtosecond hard XFEL pulse sequence.

Here we demonstrate the results of investigating the damage threshold of a LiF crystal after irradiating it with a sequence of coherent femtosecond pulses using the European X-ray Free Electron Laser (EuXFEL). The laser fluxes on the crystal surface varied in the range ∼ 0.015-13 kJ/cm2 per pulse when irradiated with a sequence of 1-100 pulses (tpulse ∼ 20 fs, Eph = 9 keV). Analysis of the surface of the irradiated crystal using different reading systems allowed the damage areas and the topology of the craters formed to be accurately determined. It was found that the ablation threshold decreases with increasing number of X-ray pulses, while the depth of the formed craters increases non-linearly and reaches several hundred nanometers. The obtained results have been compared with data already available in the literature for nano- and picosecond pulses from lasers in the soft X-ray/VUV and optical ranges. A failure model of lithium fluoride is developed and verified with simulation of material damage under single-pulse irradiation. The obtained damage threshold is in reasonably good agreement with the experimentally measured one.

Soft X-ray diffraction patterns measured by a LiF detector with sub-micrometre resolution and an ultimate dynamic range.

The unique diagnostic possibilities of X-ray diffraction, small X-ray scattering and phase-contrast imaging techniques applied with high-intensity coherent X-ray synchrotron and X-ray free-electron laser radiation can only be fully realized if a sufficient dynamic range and/or spatial resolution of the detector is available. In this work, it is demonstrated that the use of lithium fluoride (LiF) as a photoluminescence (PL) imaging detector allows measuring of an X-ray diffraction image with a dynamic range of ∼107 within the sub-micrometre spatial resolution. At the PETRA III facility, the diffraction pattern created behind a circular aperture with a diameter of 5 µm irradiated by a beam with a photon energy of 500 eV was recorded on a LiF crystal. In the diffraction pattern, the accumulated dose was varied from 1.7 × 105 J cm-3 in the central maximum to 2 × 10-2 J cm-3 in the 16th maximum of diffraction fringes. The period of the last fringe was measured with 0.8 µm width. The PL response of the LiF crystal being used as a detector on the irradiation dose of 500 eV photons was evaluated. For the particular model of laser-scanning confocal microscope Carl Zeiss LSM700, used for the readout of the PL signal, the calibration dependencies on the intensity of photopumping (excitation) radiation (λ = 488 nm) and the gain have been obtained.

Ion pinhole imaging diagnostics on fast ion source in femtosecond laser plasma of cluster targets.

The spatial configuration of the ion source generated under femtosecond laser interaction with clusters is investigated. While intense laser pulses (36 fs, 60 mJ, intensity of 4 × 1017 W/cm2) propagated in CO2 cluster (~0.22 µm in diameter) media, the shape of the obtained plasma ion source was registered for the first time by means of pinhole imaging method. The remarkable decrease in fast ion yield in the vicinity of the assumed best laser focus near the gas cluster jet axis is observed. Such observed anisotropy of the ion source is suggested to originate from the influence of the laser prepulse destroying clusters in advance to the arrival of the main pulse. The assumption is confirmed by optical shadowgraphy images of the plasma channel and is important for further development of an efficient laser-plasma-based fast ion source. Following the observed geometry of the ion source, the laser intensity limit allowing to accelerate ions to ~100 keV energy range was estimated.

Revealing the second harmonic generation in a femtosecond laser-driven cluster-based plasma by analyzing shapes of Ar XVII spectral lines.

We present experiments dealing with a femtosecond laser-driven cluster-based plasma, where by analyzing the nonlinear phenomenon of satellites of spectral lines of Ar XVII, we revealed the nonlinear phenomenon of the generation of the second harmonic of the laser frequency. For performing this analysis we developed new results in the theory of satellites of spectral lines. From such lineshape analysis we found, in particular, that the efficiency of converting the short (40 fs) intense (3x10¹8 W/cm²) incident laser light into the second harmonic was 2%. This result is in the excellent agreement with the 2-Dimensional Particle-In-Cell (2D PIC) simulation that we also performed. There is also an order of magnitude agreement between the thresholds for the SHG found from the line shape analysis and from the 2D PIC simulations.

Soft x-ray free-electron laser imaging by LiF crystal and film detectors over a wide range of fluences.

LiF crystal and film detectors were used to measure the far-field fluence profile of a self-amplified spontaneous-emission free-electron laser beam and diffraction imaging with high spatial resolution. In these measurements the photoluminescence (PL) response of LiF crystal and film was compared over a wide range of soft x-ray fluences. It was found that the soft x-ray fluence dependences of LiF crystal and film differ. At low fluence, the LiF crystal shows higher PL response compared to LiF film, while this comparison is the opposite at higher fluence. Accurate measurement of LiF crystal and film PL response is important for precise characterization of the spatial, spectral, and coherence features of x-ray beams across the full profile and in localized areas. For such measurements, crucial LiF detector attributes are high spatial resolution and high dynamic range.

Transonic dislocation propagation in diamond.

The motion of line defects (dislocations) has been studied for more than 60 years, but the maximum speed at which they can move is unresolved. Recent models and atomistic simulations predict the existence of a limiting velocity of dislocation motion between the transonic and subsonic ranges at which the self-energy of dislocation diverges, though they do not deny the possibility of the transonic dislocations. We used femtosecond x-ray radiography to track ultrafast dislocation motion in shock-compressed single-crystal diamond. By visualizing stacking faults extending faster than the slowest sound wave speed of diamond, we show the evidence of partial dislocations at their leading edge moving transonically. Understanding the upper limit of dislocation mobility in crystals is essential to accurately model, predict, and control the mechanical properties of materials under extreme conditions.

Optical features of a LiF crystal soft X-ray imaging detector irradiated by free electron laser pulses.

Optical features of point defects photoluminescence in LiF crystals, irradiated by soft X-ray pulses of the Free Electron Laser with wavelengths of 17.2 - 61.5 nm, were measured. We found that peak of photoluminescence spectra lies near of 530 nm and are associated with emission of F3+ centers. Our results suggest that redistribution of photoluminescence peak intensity from the red to the green part of the spectra is associated with a shortening of the applied laser pulses down to pico - or femtosecond durations. Dependence of peak intensity of photoluminescence spectra from the soft X-ray irradiation fluence was measured and the absence of quenching phenomena, even at relatively high fluencies was found, which is very important for wide applications of LiF crystal X-ray imaging detectors.

Enhanced Kα output of Ar and Kr using size optimized cluster target irradiated by high-contrast laser pulses.

We observed that increasing the clusters size and laser pulse contrast can enhance the X-ray flux emitted by femtosecond-laser-driven-cluster plasma. By focusing a high contrast laser (10(-10)) on large argon clusters, high flux Kα-like X-rays (around 2.96 keV) is generated with a total flux of 2.5 × 10(11) photons/J in 4π and a conversion efficiency of 1.2 × 10-4. In the case of large Kr clusters, the best total flux for L-shell X-rays is 5.3 × 1011 photons/J with a conversion efficiency of 1.3 × 10-4 and, for the Kα X-ray (12.7 keV), it is 8 × 10(8) photons/J with a conversion efficiency of 1.6 × 10-6. Using this X-ray source, a single-shot high-performance X-ray imaging is demonstrated.

Efficient generation of Xe K-shell x rays by high-contrast interaction with submicrometer clusters.

The interaction between a 25 TW laser and Xe clusters at a peak intensity of 1 × 10¹9 W/cm² has been investigated. Xe K-shell x rays, whose energies are approximately 30 keV, were clearly observed with a hard x-ray CCD at 3.4 MPa. Moreover, we studied the yield of the Xe K-shell x rays by changing the pulse duration of the laser at a constant laser energy and found that the pulse duration of 40 fs is better than that of 300 fs for generating Xe K-shell x rays.

Ultrafast olivine-ringwoodite transformation during shock compression.

Meteorites from interplanetary space often include high-pressure polymorphs of their constituent minerals, which provide records of past hypervelocity collisions. These collisions were expected to occur between kilometre-sized asteroids, generating transient high-pressure states lasting for several seconds to facilitate mineral transformations across the relevant phase boundaries. However, their mechanisms in such a short timescale were never experimentally evaluated and remained speculative. Here, we show a nanosecond transformation mechanism yielding ringwoodite, which is the most typical high-pressure mineral in meteorites. An olivine crystal was shock-compressed by a focused high-power laser pulse, and the transformation was time-resolved by femtosecond diffractometry using an X-ray free electron laser. Our results show the formation of ringwoodite through a faster, diffusionless process, suggesting that ringwoodite can form from collisions between much smaller bodies, such as metre to submetre-sized asteroids, at common relative velocities. Even nominally unshocked meteorites could therefore contain signatures of high-pressure states from past collisions.

Propagation-based phase-contrast enhancement of nanostructure images using a debris-free femtosecond-laser-driven cluster-based plasma soft x-ray source and an LiF crystal detector.

We demonstrate in-line phase-contrast imaging of nanothickness foils by using a relatively large, polychromatic, debris-free femtosecond-laser-driven cluster-based plasma soft x-ray source, and a high-resolution, large dynamic range LiF crystal detector. The spatial coherence length of radiation in our setup reached a value of 5 microm on the sample plane, which is enough to observe phase-contrast enhancement in the images registered by the detector placed only a few hundred micrometers behind the object. We have developed a tabletop soft x-ray emission source, which emits radiation within a 4pi sr solid angle, and which allows one to obtain contact and propagation-based phase-contrast imaging of nanostructures with 700 nm spatial resolutions. This advance could be of utility for metrology applications.

Modeling energy dependence of the inner-shell x-ray emission produced by femtosecond-pulse laser irradiation of xenon clusters.

We employ the Los Alamos suite of atomic physics codes to model the inner-shell x-ray emission spectrum of xenon and compare results with those obtained via high-resolution x-ray spectroscopy of xenon clusters irradiated by 30fs Ti:Sapphire laser pulses. We find that the commonly employed configuration-average approximation breaks down and significant spin-orbit splitting necessitates a detailed level accounting. We reproduce an interesting spectral trend for a series of experimental spectra taken with varying pulse energy for fixed pulse duration. To simulate the experimental measurements at increasing beam energies, we find that spectral modeling requires an increased hot electron fraction, but decreased atomic density and bulk electron temperature. We believe these latter conditions to be a result of partial cluster destruction due to the increased energy in the laser prepulse.

Qualitative detection of Mg content in a leaf of Hedera helix by using X-ray radiation from a laser plasma source.

In this article, a method to reveal the presence of Mg content inside the different parts of leaves of Hedera helix is presented. In fact a sample of a Hedera helix's leaf, commonly characterized by a green and a white side, is analyzed under X-ray radiation. The presence of two zones with different colors in the Hedera helix's leaf has not been explained. In this connection, there are presently three hypotheses to explain the characteristic double-color appearance of the leaf. The first hypothesis suggests a different cytoplasmic inheritance of chloroplasts at the cell division, the second a different allelic composition, homozygote and heterozygote, between the two zones, and finally the third the action of a virus which changes the color properties in the Hedera's leaves. The resulting effect is a different content of "something" between the green and the white side. We utilized X-ray radiation, obtained from a plasma source with a Mg target, to image Hedera helix leaves and we found that the green side of the leaf is highlighted. We may suppose that the reason why the X-rays from a Mg plasma source, allow us to pick up the green side is probably due to the greater presence of the amount of Mg (from chlorophyll or other complexes and/or salts) in the two sides, green and white, of the leaf.

Dynamic fracture of tantalum under extreme tensile stress.

The understanding of fracture phenomena of a material at extremely high strain rates is a key issue for a wide variety of scientific research ranging from applied science and technological developments to fundamental science such as laser-matter interaction and geology. Despite its interest, its study relies on a fine multiscale description, in between the atomic scale and macroscopic processes, so far only achievable by large-scale atomic simulations. Direct ultrafast real-time monitoring of dynamic fracture (spallation) at the atomic lattice scale with picosecond time resolution was beyond the reach of experimental techniques. We show that the coupling between a high-power optical laser pump pulse and a femtosecond x-ray probe pulse generated by an x-ray free electron laser allows detection of the lattice dynamics in a tantalum foil at an ultrahigh strain rate of [Formula: see text] ~2 × 108 to 3.5 × 108 s-1. A maximal density drop of 8 to 10%, associated with the onset of spallation at a spall strength of ~17 GPa, was directly measured using x-ray diffraction. The experimental results of density evolution agree well with large-scale atomistic simulations of shock wave propagation and fracture of the sample. Our experimental technique opens a new pathway to the investigation of ultrahigh strain-rate phenomena in materials at the atomic scale, including high-speed crack dynamics and stress-induced solid-solid phase transitions.

Microradiography as a tool to detect heavy metal uptake in plants for phytoremediation applications.

In this paper, an application of contact microradiography with soft X-rays for detecting the uptake site of heavy metal in the whole plant leaves is investigated. The X-ray source is a laser-plasma one based on an Nd:glass laser. The soft X-ray radiation emitted from the plasma laser targets of magnesium, iron, and copper can be strongly absorbed in the leaves' regions rich in iron, magnesium, and copper. This absorbance could point to structures in the leaves where these heavy elements are found. In this work, leaves treated with copper sulfate diluted in water at 1, 2, and 5% were imaged by using a copper target, in order to evaluate differences with untreated control leaves. Our results showed that this methodology highlighted the presence of copper in the treated leaves. This new methodology should detect heavy element pollutants inside plants and it should also be a useful analytic tool in phytoremediation studies.

3D visualization of XFEL beam focusing properties using LiF crystal X-ray detector.

Here, we report, that by means of direct irradiation of lithium fluoride a (LiF) crystal, in situ 3D visualization of the SACLA XFEL focused beam profile along the propagation direction is realized, including propagation inside photoluminescence solid matter. High sensitivity and large dynamic range of the LiF crystal detector allowed measurements of the intensity distribution of the beam at distances far from the best focus as well as near the best focus and evaluation of XFEL source size and beam quality factor M(2). Our measurements also support the theoretical prediction that for X-ray photons with energies ~10 keV the radius of the generated photoelectron cloud within the LiF crystal reaches about 600 nm before thermalization. The proposed method has a spatial resolution ~0.4-2.0 µm for photons with energies 6-14 keV and potentially could be used in a single shot mode for optimization of different focusing systems developed at XFEL and synchrotron facilities.

Observation and theory of X-ray mirages.

The advent of X-ray lasers allowed the realization of compact coherent soft X-ray sources, thus opening the way to a wide range of applications. Here we report the observation of unexpected concentric rings in the far-field beam profile at the output of a two-stage plasma-based X-ray laser, which can be considered as the first manifestation of a mirage phenomenon in X-rays. We have developed a method of solving the Maxwell-Bloch equations for this problem, and find that the experimentally observed phenomenon is due to the emergence of X-ray mirages in the plasma amplifier, appearing as phase-matched coherent virtual point sources. The obtained results bring a new insight into the physical nature of amplification of X-ray radiation in laser-induced plasma amplifiers and open additional opportunities for X-ray plasma diagnostics and extreme ultraviolet lithography.