R.A. Loch

Fixed target combined with spectral mapping: approaching 100% hit rates for serial crystallography.

The advent of ultrafast highly brilliant coherent X-ray free-electron laser sources has driven the development of novel structure-determination approaches for proteins, and promises visualization of protein dynamics on sub-picosecond timescales with full atomic resolution. Significant efforts are being applied to the development of sample-delivery systems that allow these unique sources to be most efficiently exploited for high-throughput serial femtosecond crystallography. Here, the next iteration of a fixed-target crystallography chip designed for rapid and reliable delivery of up to 11 259 protein crystals with high spatial precision is presented. An experimental scheme for predetermining the positions of crystals in the chip by means of in situ spectroscopy using a fiducial system for rapid, precise alignment and registration of the crystal positions is presented. This delivers unprecedented performance in serial crystallography experiments at room temperature under atmospheric pressure, giving a raw hit rate approaching 100% with an effective indexing rate of approximately 50%, increasing the efficiency of beam usage and allowing the method to be applied to systems where the number of crystals is limited.

Phase characterization of the reflection on an extreme UV multilayer: comparison between attosecond metrology and standing wave measurements.

We characterize the phase shift induced by reflection on a multilayer mirror in the extreme UV range (80-93 eV) using two techniques: one based on high order harmonic generation and attosecond metrology (reconstruction of attosecond beating by interference of two-photon transitions), and a second based on synchrotron radiation and measurements of standing waves (total electron yield). We find an excellent agreement between the results from the two measurements and a flat group delay shift (±40 as) over the main reflectivity peak of the mirror.

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.

Interlayer growth in Mo/B4C multilayered structures upon thermal annealing

Both multilayer period thickness expansion and compaction were observed in Mo/B4C multilayers upon annealing, and the physical causes for this were explored in detail. Using in situ timedependent grazing incidence X-ray reflectometry, period changes down to picometer-scale were resolved. It was shown that the changes depend on the thickness of the B4C layers, annealing temperature, and annealing time. Although strong stress relaxation during annealing was observed, it was excluded as a cause for period expansion. Auger electron spectroscopy and wide angle X-ray diffraction measurements revealed the growth of interlayers, with associated period changes influenced by the supply of B and C atoms to the growing compound interlayers. For multilayers with a Mo thickness of 3 nm, two regimes were recognized, depending on the deposited B4C thickness: in multilayers with B4C 1.5 nm, the supply of additional Mo into the already formed MoBxCy interlayer was dominant and led to densification, resulting in period compaction. For multilayers with B4C 2 nm, the B and C enrichment of interlayers formed low density compounds and yielded period expansion.

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.

High Reflectance Nanoscale V/Sc Multilayer for Soft X-ray Water Window Region

V/Sc multilayer is experimentally demonstrated for the first time as a high reflectance mirror for the soft X-ray water window region. It primarily works at above the Sc-L edge (λ = 3.11 nm) under near normal incidence while a second peak appears at above the V-L edge (λ = 2.42 nm) under grazing incidence. The V/Sc multilayer fabricated with a d-spacing of 1.59 nm and 30 bilayers has a smaller interface width (σ = 0.27 and 0.32 nm) than the conventional used Cr/Sc (σ = 0.28 and 0.47 nm). For V/Sc multilayer with 30 bilayers, the introduction of B4C barrier layers has little improvement on the interface structure. As the number of bilayers increasing to 400, the growth morphology and microstructure of the V/Sc layers evolves with slightly increased crystallization. Nevertheless, the surface roughness remains to be 0.25 nm. A maximum soft X-ray reflectance of 18.4% is measured at λ = 3.129 nm at 9° off-normal incidence using the 400-bilayers V/Sc multilayer. According to the fitted model, an s-polarization reflectance of 5.2% can also be expected at λ = 2.425 nm under 40° incidence. Based on the promising experimental results, further improvement of the reflectance can be achieved by using a more stable deposition system, exploring different interface engineering methods and so on.

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.

Soft X-ray Free-Electron Laser Induced Damage to Inorganic Scintillators

An irreversible response of inorganic scintillators to intense soft x-ray laser radiation was investigated at the FLASH (Free-electron LASer in Hamburg) facility. Three ionic crystals, namely, Ce:YAG (cerium-doped yttrium aluminum garnet), PbWO4 (lead tungstate), and ZnO (zinc oxide), were exposed to single 4.6 nm ultra-short laser pulses of variable pulse energy (up to 12 μJ) under normal incidence conditions with tight focus. Damaged areas produced with various levels of pulse fluences, were analyzed on the surface of irradiated samples using differential interference contrast (DIC) and atomic force microscopy (AFM). The effective beam area of 22.2 ± 2.2 μm2 was determined by means of the ablation imprints method with the use of poly(methyl methacrylate) - PMMA. Applied to the three inorganic materials, this procedure gave almost the same values of an effective area. The single-shot damage threshold fluence was determined for each of these inorganic materials. The Ce:YAG sample seems to be the most radiation resistant under the given irradiation conditions, its damage threshold was determined to be as high as 660.8 ± 71.2 mJ/cm2. Contrary to that, the PbWO4 sample exhibited the lowest radiation resistance with a threshold fluence of 62.6 ± 11.9 mJ/cm2. The threshold for ZnO was found to be 167.8 ± 30.8 mJ/cm2. Both interaction and material characteristics responsible for the damage threshold difference are discussed in the article.

Modelling single shot damage thresholds of multilayer optics for high-intensity short-wavelength radiation sources

The single shot damage thresholds of multilayer optics for high-intensity short-wavelength radiation sources are theoretically investigated, using a model developed on the basis of experimental data obtained at the FLASH and LCLS free electron lasers. We compare the radiation hardness of commonly used multilayer optics and propose new material combinations selected for a high damage threshold. Our study demonstrates that the damage thresholds of multilayer optics can vary over a large range of incidence fluences and can be as high as several hundreds of mJ/cm(2). This strongly suggests that multilayer mirrors are serious candidates for damage resistant optics. Especially, multilayer optics based on Li(2)O spacers are very promising for use in current and future short-wavelength radiation sources.

Mo/Si multilayer-coated amplitude-division beam splitters for XUV radiation sources

Short-wavelength XUV beam splitters consisting of multilayer reflective and transmissive coatings on 3 × 3 mm and 10 × 10 mm SiN membranes have been developed and fully characterized.