Contrasting behavior of covalent and molecular carbon allotropes exposed to extreme ultraviolet and soft x-ray free-electron laser radiation

All carbon materials, e.g., amorphous carbon (a-C) coatings and C60 fullerene thin films, play an important role in short-wavelength free-electron laser (FEL) research motivated by FEL optics development and prospective nanotechnology applications. Responses of a-C and C60 layers to the extreme ultraviolet (SPring-8 Compact SASE Source in Japan) and soft x-ray (free-electron laser in Hamburg) free-electron laser radiation are investigated by Raman spectroscopy, differential interference contrast, and atomic force microscopy. A remarkable difference in the behavior of covalent (a-C) and molecular (C60) carbonaceous solids is demonstrated under these irradiation conditions. Low thresholds for ablation of a fullerene crystal (estimated to be around 0.15 eV/atom for C60 vs 0.9 eV/atom for a-C in terms of the absorbed dose) are caused by a low cohesive energy of fullerene crystals. An efficient mechanism of the removal of intact C60 molecules from the irradiated crystal due to Coulomb repulsion of fullerene-cage cation radicals formed by the ionizing radiation is revealed by a detailed modeling

Study of ultrathin Pt/Co/Pt trilayers modified by nanosecond XUV pulses from laser-driven plasma source

We have studied the structural mechanisms responsible for the magnetic reorientation between in-plane and out-of-plane magnetization in the (25 nm Pt)/(3 and 10 nm Co)/(3 nm Pt) trilayer systems irradiated with nanosecond XUV pulses generated with laser-driven gas-puff target plasma source of a narrow continuous spectrum peaked at wavelength of 11 nm. The thickness of individual layers, their density, chemical composition and irradiation-induced lateral strain were deduced from symmetric and asymmetric X-ray diffraction (XRD) patterns, grazing-incidence X-ray reflectometry (GIXR), grazing incidence X-ray fluorescence (GIXRF), extended X-ray absorption fine structure (EXAFS) and transmission electron microscopy (TEM) measurements. In the as grown samples we found, that the Pt buffer layers are relaxed and that the layer interfaces are sharp. As a result of a quasi-uniform irradiation of the samples, the XRD, EXAFS, GIXR and GIXRF data reveal the formation of two distinct layers composed of Pt1-xCox alloys with different Co concentrations, dependent on the thickness of the as grown magnetic Co film but with similar ∼1% lateral tensile residual strain. For smaller exposure dose (lower number of accumulated pulses) only partial interdiffusion at the interfaces takes place with the formation of a tri-layer composed of Co-Pt alloy sandwiched between thinned Pt layers, as revealed by TEM. The structural modifications are accompanied by magnetization changes, evidenced by means of magneto-optical microscopy. The difference in magnetic properties of the irradiated samples can be related to their modification in Pt1-xCox alloy composition, as the other parameters (lateral strain and alloy thickness) remain almost unchanged. The out-of-plane magnetization observed for the sample with initially 3 nm Co layer can be due to a significant reduction of demagnetization factor resulting from a lower Co concentration

Damage accumulation in thin ruthenium films induced by repetitive exposure to femtosecond XUV pulses below the single shot ablation threshold

The process of damage accumulation in thin ruthenium films exposed to multiple femtosecond XUV free electron laser FEL pulses below the critical angle of reflectance at the Free electron LASer facility in Hamburg FLASH was experimentally analyzed. The multi shot damage threshold is found to be lower than single shot damage threshold. Detailed analysis of the damage morphology and its dependence on irradiation conditions justifies the assumption that cavitation induced by the FEL pulse is the prime mechanism responsible for multi shot damage in optical coating

Sub-nanometer-scale measurements of the interaction of ultrafast soft x-ray free-electron-laser pulses with matter

Femtosecond pulses from soft-x-ray free-electron lasers (FELs) [1] are ideal for directly probing matter at atomic length scales and timescales of atomic motion. An important component of understanding ultrafast phenomena of light-matter interactions is concerned with the onset of atomic motion which is impeded by the atoms inertia. This delay of structural changes will enable atomic-resolution flash-imaging [2-3] to be performed at upcoming x-ray FELs [4-5] with pulses intense enough to record the x-ray scattering from single molecules [6]. We explored this ultrafast high-intensity regime with the FLASH soft-x-ray FEL [7-8] by measuring the reflectance of nanostructured multilayer mirrors using pulses with fluences far in excess of the mirrors damage threshold. Even though the nanostructures were ultimately completely destroyed, we found that they maintained their integrity and reflectance characteristics during the 25-fs-long pulse, with no evidence for any structural changes during that time over lengths greater than 3 {angstrom}. In the recently built FLASH FEL [7], x-rays are produced from short electron pulses oscillating in a periodic magnet array, called an undulator, by the principle of self-amplification of spontaneous emission [9-10]. The laser quality of the x-ray pulses can be quantified by the peak spectral brilliance of the source, which is 10{sup 28} photons/(s mm2 mrad2 0.1% bandwidth) [8]; this is up to seven orders of magnitude higher than modern third-generation synchrotron sources. For our studies, the machine operated with pulses of 25 fs duration at a wavelength of 32.5 nm and energies up to 21 {micro}J. We focused these pulses to 3 x 10{sup 14} W/cm{sup 2} onto our nanostructured samples, resulting in an the unprecedented heating rate of 5 x 10{sup 18} K/s, while probing the irradiated structures at the nanometer length scale. The x-ray reflectivity of periodic nanometer-scale multilayers [11] is very sensitive to changes in the atomic positions and the refractive indices of the constituent materials, making them an ideal choice to study structural changes induced by ultrashort FEL pulses. The large multilayer reflectivity results from the cooperative interaction of the x-ray field with many layers of precisely fabricated thicknesses, each less than the x-ray wavelength. This Bragg or resonant reflection from the periodic structure is easily disrupted by any imperfection of the layers. The characteristics of the structure, such as periodicity or layer intermixing, can be precisely determined from the measurement of the Bragg reflectivity as a function of incidence angle. These parameters can be easily measured to a small fraction of the probe wavelength, as is well known in x-ray crystallography where average atomic positions of minerals or proteins are found to less than 0.01{angstrom}. Thus, we can explore ultrafast phenomena at length scales less than the wavelength, and investigate the conditions to overcome the effects of radiation damage by using ultrafast pulses

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 mode

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 morphologie

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 surfac