J. Chalupsky

Characteristics of focused soft X-ray free-electron laser beam determined by ablation of organic molecular solids

A linear accelerator based source of coherent radiation, FLASH (Free-electron LASer in Hamburg) provides ultra-intense femtosecond radiation pulses at wavelengths from the extreme ultraviolet (XUV; lambda<100nm) to the soft X-ray (SXR; lambda<30nm) spectral regions. 25-fs pulses of 32-nm FLASH radiation were used to determine the ablation parameters of PMMA - poly (methyl methacrylate). Under these irradiation conditions the attenuation length and ablation threshold were found to be (56.9+/-7.5) nm and approximately 2 mJ*cm(-2), respectively. For a second wavelength of 21.7 nm, the PMMA ablation was utilized to image the transverse intensity distribution within the focused beam at mum resolution by a method developed here.

The soft x-ray instrument for materials studies at the linac coherent light source x-ray free-electron laser.

The soft x-ray materials science instrument is the second operational beamline at the linac coherent light source x-ray free electron laser. The instrument operates with a photon energy range of 480-2000 eV and features a grating monochromator as well as bendable refocusing mirrors. A broad range of experimental stations may be installed to study diverse scientific topics such as: ultrafast chemistry, surface science, highly correlated electron systems, matter under extreme conditions, and laboratory astrophysics. Preliminary commissioning results are presented including the first soft x-ray single-shot energy spectrum from a free electron laser.

Soft x-ray free electron laser microfocus for exploring matter under extreme conditions

We have focused a beam (BL3) of FLASH (Free-electron LASer in Hamburg: lambda = 13.5 nm, pulse length 15 fs, pulse energy 10-40 microJ, 5 Hz) using a fine polished off-axis parabola having a focal length of 270 mm and coated with a Mo/Si multilayer with an initial reflectivity of 67% at 13.5 nm. The OAP was mounted and aligned with a picomotor controlled six-axis gimbal. Beam imprints on poly(methyl methacrylate) - PMMA were used to measure focus and the focused beam was used to create isochoric heating of various slab targets. Results show the focal spot has a diameter of < or =1 microm. Observations were correlated with simulations of best focus to provide further relevant information.

Interaction of short x-ray pulses with low-Z x-ray optics materials at the LCLS free-electron laser

Materials used for hard x-ray-free-electron laser (XFEL) optics must withstand high-intensity x-ray pulses. The advent of the Linac Coherent Light Source has enabled us to expose candidate optical materials, such as bulk B4C and SiC films, to 0.83 keV XFEL pulses with pulse energies between 1 μJ and 2 mJ to determine short-pulse hard x-ray damage thresholds. The fluence required for the onset of damage for single pulses is around the melt fluence and slightly lower for multiple pulses. We observed strong mechanical cracking in the materials, which may be due to the larger penetration depths of the hard x-rays.

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.

X-ray laser-induced ablation of lead compounds

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.

Experimental set-up and procedures for the investigation of XUV free electron laser interactions with solids

In this article, we describe the experimental station and procedures for investigating the interaction of short-wavelength free-electron lasers (FELs) pulses with solids. With the advent of these sources, a unique combination of radiation properties (including wavelength range from tens of nanometers down to sub-Angstroms, femtosecond pulse duration, and high pulse energy reaching milli-Joules level) creates new research possibilities for the systematic studies of radiation-induced structural changes in solids. However, the properties of the intense FEL radiation generate, apart from the new experimental opportunities, extreme demands on the experimental set-up (mostly in terms of radiation hardness of detectors and their saturation levels). Thus, radiation-induced phase transitions in solids, beyond the fundamental scientific interest, are of importance for the design of FEL beamlines and instruments which interact with the direct beam. In this report, we focus on the instrumentation and experimental techniques used in the recent studies performed at the FLASH facility in Hamburg.

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.

Enhanced surface structuring by ultrafast XUV/NIR dual action

Materials processing utilizing ultrashort near-infrared (NIR) laser pulses with duration in the range of tens to hundreds of femtoseconds (1fs = 10 15 s) has attracted a great deal of interest in the scientific and industrial world recently. Unfortunately, a number of materials that often exhibit great technological and scientific importance are transparent in NIR, making it very difficult to process them by laser radiation in this spectral range. Here, we present a new method for the efficient structuring of the surface of materials by applying femtosecond NIR laser pulses simultaneously with a weak extreme ultraviolet (XUV) beam, which leads to very strong radiation-matter interaction, bringing a dramatic increase in the surface processing speed. A laser system providing 5mJ, 820nm, 32fs, 10Hz pulses was used to generate high-order harmonics with the strongest spectral line at 21nm and with a conversion efficiency of 5%. The two beams were focused on the samples by using an off-axis paraboloidal multilayer mirror. As an example, we present the results of the surface nanostructuring of thin films of amorphous carbon and poly(methyl methacrylate) deposited on bulk substrates. We discuss the physical mechanisms that lead to the laser-induced periodic surface structures when our method is used.

Ablative microstructuring with plasma-based XUV lasers and efficient processing of materials by dual action of XUV/NIR–VIS ultrashort pulses

We report on a single-shot micropatterning of an organic polymer achieved by ablation with demagnifying projection using a plasma-based extreme ultraviolet (XUV) laser at 21 nm. A nickel mesh with a period of 100 μ m was 10×demagnified and imprinted on poly(methyl methacrylate) (PMMA) via direct ablation. This first demonstration of single-shot projection, single-step lithography illustrates the great potential of XUV lasers for the direct patterning of materials with a resolution scalable down to the submicrometer domain. In the second part, we present a novel experimental method for improving the efficiency of surface processing of various solids achieved by simultaneous action of XUV, obtained from high-order harmonic generation, and near-infrared (NIR)–VIS laser pulses. The NIR–VIS pulse interacts with free charge carriers produced by the energetic XUV photons, so that its absorption dramatically increases. Laser-induced periodic surface structures were effectively produced using this technique.