Dense plasma environment affects the electronic structure of ions via variations of the microscopic electrical fields, also known as plasma screening. This effect can be either estimated by simplified analytical models, or by computationally expensive and to date unverified numerical calculations. We have experimentally quantified plasma screening from the energy shifts of the bound-bound transitions in matter driven by the x-ray free electron laser (XFEL). This was enabled by identification of detailed electronic configurations of the observed K{\alpha}, K\b{eta} and K{\gamma} lines. This work paves the way for improving plasma screening models including connected effects like ionization potential depression and continuum lowering, which will advance the understanding of atomic physics in Warm Dense Matter regime.
X-ray free electron laser (XFEL) sources coupled to high-power laser systems offer an avenue to study the structural dynamics of materials at extreme pressures and temperatures. The recent commissioning of the DiPOLE 100-X laser on the high energy density (HED) instrument at the European XFEL represents the state-of-the-art in combining x-ray diffraction with laser compression, allowing for compressed materials to be probed in unprecedented detail. Here, we report quantitative structural measurements of molten Sn compressed to 85(5) GPa and ∼3500 K. The capabilities of the HED instrument enable liquid density measurements with an uncertainty of ∼1% at conditions which are extremely challenging to reach via static compression methods. We discuss best practices for conducting liquid diffraction dynamic compression experiments and the necessary intensity corrections which allow for accurate quantitative analysis. We also provide a polyimide ablation pressure vs input laser energy for the DiPOLE 100-X drive laser which will serve future users of the HED instrument.
AbstractH2O transforms to two forms of superionic (SI) ice at high pressures and temperatures, which contain highly mobile protons within a solid oxygen sublattice. Yet the stability field of both phases remains debated. Here, we present the results of an ultrafast X-ray heating study utilizing MHz pulse trains produced by the European X-ray Free Electron Laser to create high temperature states of H2O, which were probed using X-ray diffraction during dynamic cooling. We confirm an isostructural transition during heating in the 26-69 GPa range, consistent with the formation of SI-bcc. In contrast to prior work, SI-fcc was observed exclusively above ~50 GPa, despite evidence of melting at lower pressures. The absence of SI-fcc in lower pressure runs is attributed to short heating timescales and the pressure-temperature path induced by the pump-probe heating scheme in which H2O was heated above its melting temperature before the observation of quenched crystalline states, based on the earlier theoretical prediction that SI-bcc nucleates more readily from the fluid than SI-fcc. Our results may have implications for the stability of SI phases in ice-rich planets, for example during dynamic freezing, where the preferential crystallization of SI-bcc may result in distinct physical properties across mantle ice layers.
This work presents first insights into the dynamics of free-surface release clouds from dynamically compressed polystyrene and pyrolytic graphite at pressures up to 200 GPa, where they transform into diamond or lonsdaleite, respectively. These ejecta clouds are released into either vacuum or various types of catcher systems, and are monitored with high-speed recordings (frame rates up to 10 MHz). Molecular dynamics simulations are used to give insights to the rate of diamond preservation throughout the free expansion and the catcher impact process, highlighting the challenges of diamond retrieval. Raman spectroscopy data show graphitic signatures on a catcher plate confirming that the shock-compressed PS is transformed. First electron microscopy analyses of solid catcher plates yield an outstanding number of different spherical-like objects in the size range between ten(s) up to hundreds of nanometres, which are one type of two potential diamond candidates identified. The origin of some objects can unambiguously be assigned, while the history of others remains speculative.
A multipurpose imaging x-ray crystal spectrometer is developed for the high energy density instrument of the European X-ray Free Electron Laser. The spectrometer is designed to measure x rays in the energy range of 4-10 keV, providing high-resolution, spatially resolved spectral measurements. A toroidally bent germanium (Ge) crystal is used, allowing x-ray diffraction from the crystal to image along a one-dimensional spatial profile while spectrally resolving along the other. A detailed geometrical analysis is performed to determine the curvature of the crystal. The theoretical performance of the spectrometer in various configurations is calculated by ray-tracing simulations. The key properties of the spectrometer, including the spectral and spatial resolution, are demonstrated experimentally on different platforms. Experimental results prove that this Ge spectrometer is a powerful tool for spatially resolved measurements of x-ray emission, scattering, or absorption spectra in high energy density physics.
Experiments accessing extreme conditions at x-ray free electron lasers (XFELs) involve rapidly evolving conditions of temperature. Here, we report time-resolved, direct measurements of temperature using spectral streaked optical pyrometry of x-ray and optical laser-heated states at the High Energy Density instrument of the European XFEL. This collection of typical experiments, coupled with numerical models, outlines the reliability, precision, and meaning of time dependent temperature measurements using optical emission at XFEL sources. Dynamic temperatures above 1500 K are measured continuously from spectrally- and temporally-resolved thermal emission at 450–850 nm, with time resolution down to 10–100 ns for 1–200 μs streak camera windows, using single shot and integrated modes. Targets include zero-pressure foils free-standing in air and in vacuo, and high-pressure samples compressed in diamond anvil cell multi-layer targets. Radiation sources used are 20-fs hard x-ray laser pulses at 17.8 keV, in single pulses or 2.26 MHz pulse trains of up to 30 pulses, and 250-ns infrared laser single pulses. A range of further possibilities for optical measurements of visible light in x-ray laser experiments using streak optical spectroscopy are also explored, including for the study of x-ray induced optical fluorescence, which often appears as background in thermal radiation measurements. We establish several scenarios where combined emissions from multiple sources are observed and discuss their interpretation. Challenges posed by using x-ray lasers as non-invasive probes of the sample state are addressed.
The high-precision X-ray diffraction setup for work with diamond anvil cells (DACs) in interaction chamber 2 (IC2) of the High Energy Density instrument of the European X-ray Free-Electron Laser is described. This includes beamline optics, sample positioning and detector systems located in the multipurpose vacuum chamber. Concepts for pump–probe X-ray diffraction experiments in the DAC are described and their implementation demonstrated during the First User Community Assisted Commissioning experiment. X-ray heating and diffraction of Bi under pressure, obtained using 20 fs X-ray pulses at 17.8 keV and 2.2 MHz repetition, is illustrated through splitting of diffraction peaks, and interpreted employing finite element modeling of the sample chamber in the DAC.
High-energy and high-intensity lasers are essential for pushing the boundaries of science. Their development has allowed leaps forward in basic research areas, including laser–plasma interaction, high-energy density science, metrology, biology and medical technology. The Helmholtz International Beamline for Extreme Fields user consortium contributes and operates two high-peak-power optical lasers using the high energy density instrument at the European X-ray free electron laser (EuXFEL) facility. These lasers will be used to generate transient extreme states of density and temperature to be probed by the X-ray beam. This paper introduces the ReLaX laser, a short-pulse high-intensity Ti:Sa laser system, and discusses its characteristics as available for user experiments. It will also present the first experimental commissioning results validating its successful integration into the EuXFEL infrastructure and viability as a relativistic-intensity laser driver.
Small angle x-ray scattering (SAXS) is a well established technique to detect nanometer scale structures in matter. In a typical setup, this diagnostic uses a detector with a direct line of sight to the scattering target. However, in the harsh environment of high intensity laser interaction, intense secondary radiation and high-energy particles are generated. Such a setup would therefore suffer a significant increase of noise due to this background, which could eventually prevent such measurements. In this paper, we present a novel tool consisting of a mosaic graphite crystal that works as a mirror for the SAXS signal and allows us to position the detector behind appropriate shielding. This paper studies the performance of this mirror both by experiment at the European XFEL (X-Ray Free-Electron Laser Facility) laboratory and by simulations.
The combination of powerful optical lasers and an x-ray free-electron laser (XFEL) provides unique capabilities to study the transient behaviour of matter in extreme conditions. The high energy density science instrument (HED instrument) at the European XFEL will provide the experimental platform on which an unique x-ray source can be combined with various types of high-power optical lasers. In this paper, we highlight selected scientific examples together with the associated x-ray techniques, with particular emphasis on femtosecond (fs)-timescale pump-probe experiments. Subsequently, we present the current design status of the HED instrument, outlining how the experiments could be performed. First user experiments will start at the beginning of 2018, after which various optical lasers will be commissioned and made available to the international scientific community.
Structural, defect and magnetic properties of the TiO2:Co films are investigated. We varied the maximum Co+-implantation concentration from 0.5at.% up to 5at.%. A concentration window, which is considered as a threshold for the formation of metallic secondary phases is found. At this concentration it is also observed that the majority of the dopant atoms are incorporated into the host lattice.
The manganese induced magnetic, electrical, and structural modification in InMnP epilayers, prepared by Mn ion implantation and pulsed laser annealing, are investigated in the following work. All samples exhibit clear hysteresis loops and strong spin polarization at the Fermi level. The degree of magnetization, the Curie temperature, and the spin polarization depend on the Mn concentration. The bright-field transmission electron micrographs show that InP samples become almost amorphous after Mn implantation but recrystallize after pulsed laser annealing. We did not observe an insulator-metal transition in InMnP up to a Mn concentration of 5 at. %. Instead all InMnP samples show insulating characteristics up to the lowest measured temperature. Magnetoresistance results obtained at low temperatures support the hopping conduction mechanism in InMnP. We find that the Mn impurity band remains detached from the valence band in InMnP up to 5 at. % Mn doping. Our findings indicate that the local environment of Mn ions in InP is similar to GaMnAs, GaMnP, and InMnAs; however, the electrical properties of these Mn implanted III-V compounds are different. This is one of the consequences of the different Mn binding energy in these compounds.
Chalcogen-hyperdoped silicon shows potential applications in silicon-based infrared photodetectors and intermediate band solar cells. Due to the low solid solubility limits of chalcogen elements in silicon, these materials were previously realized by femtosecond or nanosecond laser annealing of implanted silicon or bare silicon in certain background gases. The high energy density deposited on the silicon surface leads to a liquid phase and the fast recrystallization velocity allows trapping of chalcogen into the silicon matrix. However, this method encounters the problem of surface segregation. In this paper, we propose a solid phase processing by flash-lamp annealing in the millisecond range, which is in between the conventional rapid thermal annealing and pulsed laser annealing. Flash lamp annealed selenium-implanted silicon shows a substitutional fraction of ~ 70% with an implanted concentration up to 2.3%. The resistivity is lower and the carrier mobility is higher than those of nanosecond pulsed laser annealed samples. Our results show that flash-lamp annealing is superior to laser annealing in preventing surface segregation and in allowing scalability.
The fabrication of regularly ordered Ge quantum dot arrays on Si surfaces usually requires extensive preparation processing, ensuring clean and atomically ordered substrates, while the ordering parameters are quite limited by the surface properties of the substrate. Here, we demonstrate a simple method for fabrication of ordered Ge quantum dots with highly tunable ordering parameters on rippled Si surfaces. The ordering is achieved by magnetron sputter deposition, followed by an annealing in high vacuum. We show that the type of ordering and lattice vector parameters of the formed Ge quantum dot lattice are determined by the crystallographic properties of the ripples, i.e., by their shape and orientation. Moreover, the ordering is achieved regardless the initial amorphisation of the ripples surface and the presence of a thin oxide layer.
Gallium nitride is studied at ambient and nonambient temperatures by powder X‐ray diffraction followed by Rietveld refinement of the structure. The structure is reported for the ambient temperature on the basis of laboratory data. The diffraction data collected using a synchrotron beam serve for derivation of the lattice parameter and thermal expansion dependencies on temperature. The variation of unit‐cell size on temperature was studied in detail in a broad range 11 K < T < 1073 K. The obtained dependencies of a, c and V and thermal expansion coefficients are smooth, and the results are consistent with previously collected data. The c/a ratio shows an almost linear decreasing trend with rising temperature. The magnitude of thermal expansion obtained in the described experiments is similar to a recently reported theoretical one. Copyright © 2015 John Wiley & Sons, Ltd.
Amorphous, polycrystalline anatase and epitaxial anatase TiO2 films have been implanted with 5 at. % Co+. The magnetic and structural properties of different microstructures of TiO2:Co, along with the local coordination of the implanted Co atoms within the host lattice are investigated. In amorphous TiO2:Co film, Co atoms are in the (II) oxidation state with a complex coordination and exhibit a paramagnetic response. However, for the TiO2:Co epitaxial and polycrystalline anatase films, Co atoms have a distorted octahedral (II) oxygen coordination assigned to a substitutional environment with traces of metallic Co clusters, which gives a rise to a superparamagnetic behavior. Despite the incorporation of the implanted atoms into the host lattice, high temperature ferromagnetism is absent in the films. On the other hand, it is found that the concentration and size of the implantation-induced nanoclusters and the magnetic properties of TiO2:Co films have a strong dependency on the initial microstructure of TiO2. Consequently, metallic nanocluster formation within ion implantation prepared transition metal doped TiO2 can be suppressed by tuning the film microstructure.
We report effect of the initial structural order on the resulting magnetic properties of manganese implanted TiO2 films. Different microstructures of as-grown TiO2 films, namely, amorphous, polycrystalline anatase, and epitaxial anatase, have been implant-doped with Mn+ up to a concentration of 5 at. %. We found that different initial structures lead to different defect and charge carrier concentrations and, as a result, strongly influence the magnetic properties upon implantation. Depending on the initial microstructure, paramagnetism, secondary phases related magnetic properties as well as ferromagnetism could be observed in the films.
We report the structural properties of thin magnetic Permalloy films treated by two different methods: broad beam Ga+ ion implantation at an energy of 30keV as well as annealing at different temperatures under ultrahigh vacuum. Transmission electron microscopy imaging and X-ray diffraction measurements have demonstrated that both ion implantation and annealing (above 300°C) lead to further material crystallization and crystallite growth. Whereas annealing (above 400°C) leads to a strain-free state with an almost constant lattice parameter and to a further enhancement of the initial (111) texture, ion beam implantation boosts the growth of small, arbitrarily oriented crystallites and leads to an linear increase in the lattice parameter, introducing microstrain into the sample. The observed decrease in the saturation magnetization for the implanted samples is mainly attributed to the presence of the non-magnetic Ga atoms incorporated in the Permalloy film itself. The increase in the saturation magnetization for the samples annealed at temperatures above 500°C is explained by an arising dewetting effect since no ordered Ni3Fe phase was detected with anomalous X-ray diffraction.
The tunable bandgap and the high carrier mobility of Ge1−xSnx alloys stimulate a large effort for bandgap and strain engineering for Ge based materials using silicon compatible technology. In this Letter, we present the fabrication of highly mismatched Ge1−xSnx alloys by ion implantation and pulsed laser melting with Sn concentration ranging from 0.5 at. % up to 1.5 at. %. According to the structural investigations, the formed Ge1−xSnx alloys are monocrystalline with high Sn-incorporation rate. The shrinkage of the bandgap of Ge1−xSnx alloys with increasing Sn content is proven by the red-shift of the E1 and E1 + Δ1 critical points in spectroscopic ellipsometry. Our investigation provides a chip technology compatible route to prepare high quality monocrystalline Ge1−xSnx alloys.