These proceedings investigate the ionization and temperature dynamics of water samples exposed to intense ultrashort X-ray free-electron laser pulses ranging from 104 -107 J/cm2, based on simulations using a non-local thermodynamic plasma code. In comparison to earlier work combining simulations and experiments, a regime where a hybrid simulations approach should be applicable is presented.
KEYWORDS: Physics, Stanford Linear Collider, Free electron lasers, Lead, Photons, States of matter, Materials processing, Electrons, Analytical research, Raman spectroscopy
Interaction of short-wavelength free-electron laser (FEL) beams with matter is undoubtedly a subject to extensive investigation in last decade. During the interaction various exotic states of matter, such as warm dense matter, may exist for a split second. Prior to irreversible damage or ablative removal of the target material, complicated electronic processes at the atomic level occur. As energetic photons impact the target, electrons from inner atomic shells are almost instantly photo-ionized, which may, in some special cases, cause bond weakening, even breaking of the covalent bonds, subsequently result to so-called non-thermal melting. The subject of our research is ablative damage to lead tungstate (PbWO4) induced by focused short-wavelength FEL pulses at different photon energies. Post-mortem analysis of complex damage patterns using the Raman spectroscopy, atomic-force (AFM) and Nomarski (DIC) microscopy confirms an existence of non-thermal melting induced by high-energy photons in the ionic monocrystalline target. Results obtained at Linac Coherent Light Source (LCLS), Free-electron in Hamburg (FLASH), and SPring-8 Compact SASE Source (SCSS) are presented in this Paper.
N. Tîmneanu, B. Iwan, J. Andreasson, M. Bergh, M. Seibert, C. Bostedt, S. Schorb, H. Thomas, D. Rupp, T. Gorkhover, M. Adolph, T. Möller, A. Helal, K. Hoffmann, N. Kandadai, J. Keto, T. Ditmire
Understanding the ultrafast dynamics of matter under extreme conditions is relevant for structural studies and plasma physics with X-ray lasers. We used the pulses from free-electron lasers (FLASH in Hamburg and LCLS in Stanford) to trigger X-ray induced explosions in atomic atoms (Xe) and molecular clusters (CH4 and CD4). The explosion dynamics depends on cluster size and the intensity of the X-ray pulse, and a transition from Coulomb explosion to hydrodynamic expansion is expected with increasing size and increasing pulse intensity. In methane clusters experiments at FLASH, the time-of-flight spectrometry shows the appearance of molecular adducts which are the result of molecular recombination between ions and molecules. The recombination depends on the cluster size and the expansion mechanism and becomes significant in larger clusters. In Xenon cluster experiments at the LCLS, measurements of the ion charge states in clusters suggest a formation of Xe nanoplasma which expands hydrodynamically. The dominance of low charge states of Xe is due to three-body recombination processes involving electron and Xe ions, and it depends on the X-ray intensity and nanoplasma formation.
X-ray free-electron lasers enable high-resolution imaging of biological materials by using short enough pulses to outrun many of the effects of radiation damage. Experiments conducted at the LCLS have obtained diffraction data from single particles and protein nanocrystals at doses to the sample over 3 GGy. The details of the interaction of the X-ray FEL pulse with the sample determine the limits of this new paradigm for imaging. Recent studies suggest that in the case of crystalline samples, such as protein nanocrystals, the atomic displacements and loss of bound electrons in the crystal (due to the high X- ray intensity) has the effect of gating the diffraction signal, and hence making the experiment less radiation sensitive. Only the incident photon intensity in the first part of the pulse, before the Bragg diffraction has died out, is relevant to acquiring signal and the rest of the pulse will mainly contribute to a diffuse background. In this work we use a plasma based non-local thermodynamic equilibrium code to explore the displacement and the ionization of a protein nanocrystal at various X-ray wavelengths and intensities.
The recent commissioning of a X-ray free-electron laser triggered an extensive research in the area of X-ray ablation of
high-Z, high-density materials. Such compounds should be used to shorten an effective attenuation length for obtaining
clean ablation imprints required for the focused beam analysis. Compounds of lead (Z=82) represent the materials of first
choice. In this contribution, single-shot ablation thresholds are reported for PbWO4 and PbI2 exposed to ultra-short
pulses of extreme ultraviolet radiation and X-rays at FLASH and LCLS facilities, respectively. Interestingly, the
threshold reaches only 0.11 mJ/cm2 at 1.55 nm in lead tungstate although a value of 0.4 J/cm2 is expected according to
the wavelength dependence of an attenuation length and the threshold value determined in the XUV spectral region, i.e.,
79 mJ/cm2 at a FEL wavelength of 13.5 nm. Mechanisms of ablation processes are discussed to explain this discrepancy.
Lead iodide shows at 1.55 nm significantly lower ablation threshold than tungstate although an attenuation length of the
radiation is in both materials quite the same. Lower thermal and radiation stability of PbI2 is responsible for this finding.
Powerful free electron lasers (FELs) operating in the soft X-ray regime are offering new possibilities for creating
and probing materials under extreme conditions. We describe here simulations to model the interaction of a
focused FEL pulse with metallic solids (niobium, vanadium, and their deuterides) at 13.5 nm wavelength (92 eV)
with peak intensities between 1015 to 1018 W/cm2 and a fixed pulse length of 15 femtoseconds (full width at half
maximum). The interaction of the pulse with the metallic solids was modeled with a non-local thermodynamic
equilibrium code that included radiation transfer. The calculations also made use of a self-similar isothermal fluid
model for plasma expansion into vacuum. We find that the time-evolution of the simulated critical charge density
in the sample results in a critical depth that approaches the observed crater depths in an earlier experiment
performed at the FLASH free electron laser in Hamburg. The results show saturation in the ablation process
at intensities exceeding 1016 W/cm2. Furthermore, protons and deuterons with kinetic energies of several keV
have been measured, and these concur with predictions from the plasma expansion model. The results indicate
that the temperature of the plasma reached almost 5 million K after the pulse has passed.
The beam of Free-Electron Laser in Hamburg (FLASH) tuned at either 32.5 nm or 13.7 nm was focused by a grazing
incidence elliptical mirror and an off-axis parabolic mirror coated by Si/Mo multilayer on 20-micron and 1-micron spot,
respectively. The grazing incidence and normal incidence focusing of ~10-fs pulses carrying an energy of 10 μJ lead at
the surface of various solids (Si, Al, Ti, Ta, Si3N4, BN, a-C/Si, Ni/Si, Cr/Si, Rh/Si, Ce:YAG, poly(methyl methacrylate)
- PMMA, stainless steel, etc.) to an irradiance of 1013 W/cm2 and 1016 W/cm2, respectively. The optical emission of the
plasmas produced under these conditions was registered by grating (1200 lines/mm and/or 150 lines/mm) spectrometer
MS257 (Oriel) equipped with iCCD head (iStar 720, Andor). Surprisingly, only lines belonging to the neutral atoms
were observed at intensities around 1013 W/cm2. No lines of atomic ions have been identified in UV-vis spectra emitted
from the plasmas formed by the FLASH beam focused in a 20-micron spot. At intensities around 1016 W/cm2, the OE
spectra are again dominated by the atomic lines. However, a weak emission of Al+ and Al2+ was registered as well. The
abundance ratio of Al/Al+ should be at least 100. The plasma is really cold, an excitation temperature equivalent to 0.8 eV was found by a computer simulation of the aluminum plasma OE spectrum. A broadband emission was also
registered, both from the plasmas (typical is for carbon; there were no spectral lines) and the scintillators (on Ce:YAG
crystal, both the luminescence bands and the line plasma emission were recorded by the spectrometer).
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