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Inner-shell [Formula: see text] X-ray lasers have been created by pumping gaseous, solid, and liquid targets with the intense X-ray output of free-electron lasers (FELs). For gaseous targets lasing relies on the creation of [Formula: see text]-shell core holes on a time-scale short compared with filling via Auger decay. In the case of solid and liquid density systems, collisional effects will also be important, affecting not only populations but also line-widths, both of which impact the degree of overall gain, and its duration. However, to date, such collisional effects have not been extensively studied. We present here initial simulations using the CCFLY code of inner-shell lasing in solid-density Mg, where we self-consistently treat the effects of the incoming FEL radiation and the atomic kinetics of the Mg system, including radiative, Auger and collisional effects. We find that the combination of collisional population of the lower states of the lasing transitions and broadening of the lines precludes lasing on all but the [Formula: see text] of the initially cold system. Even assuming instantaneous turning on of the FEL pump, we find the duration of the gain in the solid system to be sub-femtosecond. This article is part of the theme issue 'Dynamic and transient processes in warm dense matter'.
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There is a fundamental interest in studying photoinduced dynamics in nanoparticles and nanostructures as it provides insight into their mechanical and thermal properties out of equilibrium and during phase transitions. Nanoparticles can display significantly different properties from the bulk, which is due to the interplay between their size, morphology, crystallinity, defect concentration, and surface properties. Particularly interesting scenarios arise when nanoparticles undergo phase transitions, such as melting induced by an optical laser. Current theoretical evidence suggests that nanoparticles can undergo reversible nonhomogenous melting with the formation of a core-shell structure consisting of a liquid outer layer. To date, studies from ensembles of nanoparticles have tentatively suggested that such mechanisms are present. Here we demonstrate imaging transient melting and softening of the acoustic phonon modes of an individual gold nanocrystal, using an X-ray free electron laser. The results demonstrate that the transient melting is reversible and nonhomogenous, consistent with a core-shell model of melting. The results have implications for understanding transient processes in nanoparticles and determining their elastic properties as they undergo phase transitions.
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Ionization is a problematic quantity in that it does not have a well-defined thermodynamic definition and yet it is a key parameter within plasma modeling. One still therefore aims to find a consistent and unambiguous definition for the ionization state. Within this context we present finite-temperature density functional theory calculations of the ionization state of carbon in CH plasmas using two potential definitions: one based on counting the number of continuum electrons, and another based on the optical conductivity. Differences of up to 10% are observed between the two methods. However, including "Pauli forbidden" transitions in the conductivity reproduces the counting definition, suggesting such transitions are important to evaluate the ionization state.
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We present experimental observations of K_{ß} emission from highly charged Mg ions at solid density, driven by intense x rays from a free electron laser. The presence of K_{ß} emission indicates the n=3 atomic shell is relocalized for high charge states, providing an upper constraint on the depression of the ionization potential. We explore the process of state relocalization in dense plasmas from first principles using finite-temperature density functional theory alongside a wave-function localization metric, and find excellent agreement with experimental results.
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Understanding high-velocity impact, and the subsequent high strain rate material deformation and potential catastrophic failure, is of critical importance across a range of scientific and engineering disciplines that include astrophysics, materials science, and aerospace engineering. The deformation and failure mechanisms are not thoroughly understood, given the challenges of experimentally quantifying material evolution at extremely short time scales. Here, copper foils are rapidly strained via picosecond laser ablation and probed in situ with femtosecond x-ray free electron (XFEL) pulses. Small-angle x-ray scattering (SAXS) monitors the void distribution evolution, while wide-angle scattering (WAXS) simultaneously determines the strain evolution. The ability to quantifiably characterize the nanoscale during high strain rate failure with ultrafast SAXS, complementing WAXS, represents a broadening in the range of science that can be performed with XFEL. It is shown that ultimate failure occurs via void nucleation, growth, and coalescence, and the data agree well with molecular dynamics simulations.
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In an article entitled A new theory for X-ray diffraction [Fewster (2014). Acta Cryst. A70, 257-282], hereafter referred to as NTXRD, it is claimed that when X-rays are scattered from a small crystallite, whatever its size and shape, the diffraction pattern will contain enhanced scattering at angles of exactly 2θB, whatever the orientation of the crystal. It is claimed that in this way scattering from a powder, with randomly oriented crystals, gives rise to Bragg scattering even if the Bragg condition is never satisfied by an individual crystallite. The claims of the theory put forward in NTXRD are examined and they are found to be in error. Whilst for a certain restricted set of shapes of crystals it is possible to obtain some diffraction close to (but not exactly at) the Bragg angle as the crystallite is oriented away from the Bragg condition, this is generally not the case. Furthermore, contrary to the claims made within NTXRD, the recognition of the origin of the type of effects described is not new, and has been known since the earliest days of X-ray diffraction.
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In situ white light Laue diffraction has been successfully used to interrogate the structure of single crystal materials undergoing rapid (nanosecond) dynamic compression up to megabar pressures. However, information on strain state accessible via this technique is limited, reducing its applicability for a range of applications. We present an extension to the existing Laue diffraction platform in which we record the photon energy of a subset of diffraction peaks. This allows for a measurement of the longitudinal and transverse strains in situ during compression. Consequently, we demonstrate measurement of volumetric compression of the unit cell, in addition to the limited aspect ratio information accessible in conventional white light Laue. We present preliminary results for silicon, where only an elastic strain is observed. VISAR measurements show the presence of a two wave structure and measurements show that material downstream of the second wave does not contribute to the observed diffraction peaks, supporting the idea that this material may be highly disordered, or has undergone large scale rotation.
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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.
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An extension of the time-dependent Takagi-Taupin theory to 'optical phonon'-type distortions is presented. By splitting the susceptibility into the contributions from each atom in a unit cell, modifications to the structure factor as well as lattice parameter are taken into account. The result is a compact, surprisingly simple, equation with a strong formal similarity to the classical Takagi-Taupin equation, with the latter included as a special case. Time dependence is explicitly retained and thus the analysis is applicable to situations where the crystal is modified on time scales comparable with that for the X-rays to traverse an extinction depth. A comparison is made between the influence of coherent acoustic and optical phonons on the diffraction of X-rays. Numerical and perturbative analytical solutions of the generalized Takagi-Taupin equation are presented in the presence of such phonons.
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With the pressure range accessible to laser driven compression experiments on solid material rising rapidly, new challenges in the diagnosis of samples in harsh laser environments are emerging. When driving to TPa pressures (conditions highly relevant to planetary interiors), traditional x-ray diffraction techniques are plagued by increased sources of background and noise, as well as a potential reduction in signal. In this paper we present a new diffraction diagnostic designed to record x-ray diffraction in low signal-to-noise environments. By utilising single photon counting techniques we demonstrate the ability to record diffraction patterns on nanosecond timescales, and subsequently separate, photon-by-photon, signal from background. In doing this, we mitigate many of the issues surrounding the use of high intensity lasers to drive samples to extremes of pressure, allowing for structural information to be obtained in a regime which is currently largely unexplored.
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Under uniaxial high-stress shock compression it is believed that crystalline materials undergo complex, rapid, micro-structural changes to relieve the large applied shear stresses. Diagnosing the underlying mechanisms involved remains a significant challenge in the field of shock physics, and is critical for furthering our understanding of the fundamental lattice-level physics, and for the validation of multi-scale models of shock compression. Here we employ white-light X-ray Laue diffraction on a nanosecond timescale to make the first in situ observations of the stress relaxation mechanism in a laser-shocked crystal. The measurements were made on single-crystal copper, shocked along the [001] axis to peak stresses of order 50 GPa. The results demonstrate the presence of stress-dependent lattice rotations along specific crystallographic directions. The orientation of the rotations suggests that there is double slip on conjugate systems. In this model, the rotation magnitudes are consistent with defect densities of order 10(12) cm(-2).
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The propagation of shock waves through polycrystalline iron is explored by large-scale atomistic simulations. For large enough shock strengths the passage of the wave causes the body-centered-cubic phase to transform into a close-packed phase with most structure being isotropic hexagonal-close-packed (hcp) and, depending on shock strength and grain orientation, some fraction of face-centered-cubic (fcc) structure. The simulated shock Hugoniot is compared to experiments. By calculating the extended x-ray absorption fine structure (EXAFS) directly from the atomic configurations, a comparison to experimental EXAFS measurements of nanosecond-laser shocks shows that the experimental data is consistent with such a phase transformation. However, the atomistically simulated EXAFS spectra also show that an experimental distinction between the hcp or fcc phase is not possible based on the spectra alone.