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.

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.

Real-time spatial characterization of micrometer-sized X-ray free-electron laser beams focused by bendable mirrors.

A real-time and accurate characterization of the X-ray beam size is essential to enable a large variety of different experiments at free-electron laser facilities. Typically, ablative imprints are employed to determine shape and size of µm-focused X-ray beams. The high accuracy of this state-of-the-art method comes at the expense of the time required to perform an ex-situ image analysis. In contrast, diffraction at a curved grating with suitably varying period and orientation forms a magnified image of the X-ray beam, which can be recorded by a 2D pixelated detector providing beam size and pointing jitter in real time. In this manuscript, we compare results obtained with both techniques, address their advantages and limitations, and demonstrate their excellent agreement. We present an extensive characterization of the FEL beam focused to ≈1 µm by two Kirkpatrick-Baez (KB) mirrors, along with optical metrology slope profiles demonstrating their exceptionally high quality. This work provides a systematic and comprehensive study of the accuracy provided by curved gratings in real-time imaging of X-ray beams at a free-electron laser facility. It is applied here to soft X-rays and can be extended to the hard X-ray range. Furthermore, curved gratings, in combination with a suitable detector, can provide spatial properties of µm-focused X-ray beams at MHz repetition rate.

Microscopic Kinetics in Poly(Methyl Methacrylate) Exposed to a Single Ultra-Short XUV/X-ray Laser Pulse.

We study the behavior of poly(methyl methacrylate) (PMMA) exposed to femtosecond pulses of extreme ultraviolet and X-ray laser radiation in the single-shot damage regime. The employed microscopic simulation traces induced electron cascades, the thermal energy exchange of electrons with atoms, nonthermal modification of the interatomic potential, and a triggered atomic response. We identify that the nonthermal hydrogen decoupling triggers ultrafast fragmentation of PMMA strains at the absorbed threshold dose of ~0.07 eV/atom. At higher doses, more hydrogen atoms detach from their parental molecules, which, at the dose of ~0.5 eV/atom, leads to a complete separation of hydrogens from carbon and oxygen atoms and fragmentation of MMA molecules. At the dose of ~0.7 eV/atom, the band gap completely collapses indicating that a metallic liquid is formed with complete atomic disorder. An estimated single-shot ablation threshold and a crater depth as functions of fluence agree well with the experimental data collected.

Characterization of megahertz X-ray laser beams by multishot desorption imprints in PMMA.

Proper diagnostics of intense free-electron laser (FEL) X-ray pulses is indisputably important for experimental data analysis as well as for the protection of beamline optical elements. New challenges for beam diagnostic methods are introduced by modern FEL facilities capable of delivering powerful pulses at megahertz (MHz) repetition rates. In this paper, we report the first characterization of a defocused MHz 13.5-nm beam generated by the free-electron laser in Hamburg (FLASH) using the method of multi-pulse desorption imprints in poly(methyl methacrylate)(PMMA). The beam fluence profile is reconstructed in a novel and highly accurate way that takes into account the nonlinear response of material removal to total dose delivered by multiple pulses. The algorithm is applied to experimental data of single-shot ablation imprints and multi-shot desorption imprints at both low (10 Hz) and high (1 MHz) repetition rates. Reconstructed response functions show a great agreement with the theoretical desorption response function model.

Mechanism of single-shot damage of Ru thin films irradiated by femtosecond extreme UV free-electron laser.

Ruthenium is a perspective material to be used for XUV mirrors at free-electron laser facilities. Yet, it is still poorly studied in the context of ultrafast laser-matter interaction. In this work, we present single-shot damage studies of thin Ru films irradiated by femtosecond XUV free-electron laser pulses at FLASH. Ex-situ analysis of the damaged spots, performed by different types of microscopy, shows that the weakest detected damage is surface roughening. For higher fluences we observe ablation of Ru. Combined simulations using Monte-Carlo code XCASCADE(3D) and the two-temperature model reveal that the damage mechanism is photomechanical spallation, similar to the case of irradiating the target with optical lasers. The analogy with the optical damage studies enables us to explain the observed damage morphologies.

Experimental study of EUV mirror radiation damage resistance under long-term free-electron laser exposures below the single-shot damage threshold.

The durability of grazing- and normal-incidence optical coatings has been experimentally assessed under free-electron laser irradiation at various numbers of pulses up to 16 million shots and various fluence levels below 10% of the single-shot damage threshold. The experiment was performed at FLASH, the Free-electron LASer in Hamburg, using 13.5 nm extreme UV (EUV) radiation with 100 fs pulse duration. Polycrystalline ruthenium and amorphous carbon 50 nm thin films on silicon substrates were tested at total external reflection angles of 20° and 10° grazing incidence, respectively. Mo/Si periodical multilayer structures were tested in the Bragg reflection condition at 16° off-normal angle of incidence. The exposed areas were analysed post-mortem using differential contrast visible light microscopy, EUV reflectivity mapping and scanning X-ray photoelectron spectroscopy. The analysis revealed that Ru and Mo/Si coatings exposed to the highest dose and fluence level show a few per cent drop in their EUV reflectivity, which is explained by EUV-induced oxidation of the surface.

Role of heat accumulation in the multi-shot damage of silicon irradiated with femtosecond XUV pulses at a 1 MHz repetition rate.

The role played by heat accumulation in multi-shot damage of silicon was studied. Bulk silicon samples were exposed to intense XUV monochromatic radiation of a 13.5 nm wavelength in a series of 400 femtosecond pulses, repeated with a 1 MHz rate (pulse trains) at the FLASH facility in Hamburg. The observed surface morphological and structural modifications are formed as a result of sample surface melting. Modifications are threshold dependent on the mean fluence of the incident pulse train, with all threshold values in the range of approximately 36-40 mJ/cm2. Experimental data is supported by a theoretical model described by the heat diffusion equation. The threshold for reaching the melting temperature (45 mJ/cm2) and liquid state (54 mJ/cm2), estimated from this model, is in accordance with experimental values within measurement error. The model indicates a significant role of heat accumulation in surface modification processes.

Fluence scan: an unexplored property of a laser beam.

We present an extended theoretical background of so-called fluence scan (f-scan or F-scan) method, which is frequently being used for offline characterization of focused short-wavelength (EUV, soft X-ray, and hard X-ray) laser beams [J. Chalupský et al., Opt. Express 18, 27836 (2010)]. The method exploits ablative imprints in various solids to visualize iso-fluence beam contours at different fluence and/or clip levels. An f-scan curve (clip level as a function of the corresponding iso-fluence contour area) can be generated for a general non-Gaussian beam. As shown in this paper, fluence scan encompasses important information about energy distribution within the beam profile, which may play an essential role in laser-matter interaction research employing intense non-ideal beams. Here we for the first time discuss fundamental properties of the f-scan function and its inverse counterpart (if-scan). Furthermore, we extensively elucidate how it is related to the effective beam area, energy distribution, and to the so called Liu's dependence [J. M. Liu, Opt. Lett. 7, 196 (1982)]. A new method of the effective area evaluation based on weighted inverse f-scan fit is introduced and applied to real data obtained at the SCSS (SPring-8 Compact SASE Source) facility.

Investigating the interaction of x-ray free electron laser radiation with grating structure.

The interaction of free electron laser pulses with grating structure is investigated using 4.6±0.1 nm radiation at the FLASH facility in Hamburg. For fluences above 63.7±8.7 mJ/cm2, the interaction triggers a damage process starting at the edge of the grating structure as evidenced by optical and atomic force microscopy. Simulations based on solution of the Helmholtz equation demonstrate an enhancement of the electric field intensity distribution at the edge of the grating structure. A procedure is finally deduced to evaluate damage threshold.

Linac Coherent Light Source soft x-ray materials science instrument optical design and monochromator commissioning.

We present the x-ray optical design of the soft x-ray materials science instrument at the Linac Coherent Light Source, consisting of a varied line-spaced grating monochromator and Kirkpatrick-Baez refocusing optics. Results from the commissioning of the monochromator are shown. A resolving power of 3000 was achieved, which is within a factor of two of the design goal.