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Physical review applied 14(3), 034057 (2020). doi:10.1103/PhysRevApplied.14.034057, Solids irradiated by energetic photons can be eroded in two modes, depending on the radiation intensity. High average, low-peak power sources, e.g., synchrotron radiation and high-order harmonics, induce desorption of the material at a low etch rate. In contrast, high-peak-power radiation from extreme ultraviolet and x-ray lasers usually causes a massive removal of the material even by a single shot. In this contribution, an effective material erosion is reported in PMMA exposed to multiple accumulated pulses generated by the free-electron x-ray-laser Linac Coherent Light Source (LCLS, tuned at a photon energy of 830 eV in this study, operated in Menlo Park at Stanford, CA, USA) at a fluence below the single-pulse ablation threshold. The effect is caused by polymer-chain scissions initiated by single photons carrying enough energy to break the C$—$C bounds. High efficiency of the erosion is supposed to occur due to a correlation of the single-photon effects. The subthreshold damage exhibits a nonlinear dose dependence resulting from a competition between chain scissions and cross-linking processes. The cross-linking is proven by Raman spectroscopy of the irradiated polymer. Two theoretical models of the x-ray free-electron-laser-induced erosion are suggested, which provide an excellent agreement with the experimental results., Published by American Physical Society, College Park, Md. [u.a.]

Time-resolved luminescence spectroscopy has been widely used in studies of electronic excitations and their dynamics in insulators. Present paper discusses the potential of vacuum ultraviolet spectroscopy applied for wide band gap crystals using classical synchrotron radiation as well as more recently developed pulsed femtosecond short-wavelength light sources. Optical spectroscopy using novel free electron lasers and laser systems based on higher harmonic generation process allow detailed investigation of the interaction between electronic excitations and behaviour of solids under extreme radiation conditions. Significant changes in the quantum yield and emission decay kinetics as well as surface damage of single crystals were observed for CdWO4 and CaWO4 crystals studied in the temperature range of 8-300 K. However, in the range of excitation densities applied, up to ∼1012 W/cm2, the nature of luminescence centres and their characteristic emission spectra remained similar to those observed at low excitation densities. (© 2007 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim)

International audience; Free electron lasers (FEL) are new generation accelerator-based short wavelength light sources providing high pulse intensity and femtosecond pulse duration, which enable investigation of interaction of elementary excitations in solids under extreme conditions. Using the FLASH facility of HASYLAB at DESY (Hamburg, Germany), we investigated the response of different materials with scintillating properties based on intrinsic emissions to the 25.6 and 13.8 nm FEL radiation by means of time-resolved luminescence spectroscopy. FLASH delivered single pulses of 25 fs duration having energy per pulse up to 30 μJ resulting in power densities of 1012 W/cm2 on crystals. As a function of excitation density we observed the shortening of lifetime and non-exponential behaviour of emission decays in CaWO4, while the emission spectra recorded are comparable to those obtained at conventional excitation sources

The recent development of intense sources in the XUV range (10-100 nm), such as X-ray laser, Free Electron Laser and High order Harmonics (HoH), allows the study of high flux processes and ultra-fast dynamics in various domains. At the SLIC facility of CEA-Saclay, we have built a gas-harmonic beamline to investigate the interaction of intense XUV pulse with solids. High Harmonics of an IR laser (Ti:Sa at 800 nm, 35 fs, 13 mJ/pulse, 1 kHz) are generated in a rare gas cell (Xe). The useful XUV range (40-60 nm) is selected with metallic filters. The harmonic beam is focused with a parabolic mirror to a 10 μm focal spot on sample, leading to a fluence per shot of up to 1 mJ/cm 2 (within a typical 10 fs pulse duration). Studies aimed at understanding the damaging mechanisms caused by XUV irradiation on surface of various samples by systematically varying of fluence and exposure time. For PMMA irradiated in the desorption regime (fluence/shot ≤ 0.2 mJ/cm2), the surface presents craters whose profile depends on the dose (Grey [Gy] = 1 J/kg). The crater evolution proceeds from the competition between two main degradation processes, that is chain scission and cross linking. Namely, at low dose (≤ 1 GGy) polymer chain scission is followed by the blow up of the volatile, molecular fragments, forming the crater. At high dose (> 10 GGy) the broken chain-ends, in the near-surface layer of the remaining material, recombine by cross-linking, opposing desorption by surface hardening. In a recent experiment at LCLS FEL facility, PMMA was irradiated at high fluence; the cross-linking signature was identified from Raman spectroscopy. A kinetic model could be adapted for interpreting these original and very promising results.

Exciton-exciton interaction is experimentally revealed and quantitatively analyzed in a wide band-gap scintillator material ${\text{CdWO}}_{4}$. Under high-intensity femtosecond vacuum ultraviolet excitation, the ${\text{CdWO}}_{4}$ luminescence is quenched, while its decay becomes essentially nonexponential. We propose an analytical model, which successfully reproduces the decay kinetics recorded in a wide range of excitation densities. The dipole-dipole interaction between excitons leading to their nonradiative decay is shown to be the main cause of a nonproportional response common for many scintillators.