Nanometer flat blazed x-ray gratings using ion beam figure correction.

With the development of nanometer accuracy stitching interferometry, ion beam figuring (IBF) of x-ray mirrors can now be achieved with unprecedented performance. However, the process of producing x-ray diffraction gratings on these surfaces may degrade the figure quality due to process errors introduced during the ruling of the grating grooves. To address this challenge, we have investigated the post-production correction of gratings using IBF, where stitching interferometry is used to provide in-process feedback. A concern with ion beam correction in this case is that ions will induce enough surface mobility of atoms to cause smoothing of the grating structure and degradation of diffraction efficiency. In this study we found however that it is possible to achieve a nanometer-level planarity of the global grating surface with IBF, while preserving the grating structure. The preservation was so good, that we could not detect a change in the diffraction efficiency after ion beam correction. This is of major importance in achieving ultra-high spectral resolution, and the preservation of brightness for coherent x-ray beams.

6000 lines/mm blazed grating for a high-resolution x-ray spectrometer.

We have designed and fabricated a high groove density blazed grating for a Resonant Inelastic X-ray Scattering spectrometer for the new Qerlin beamline at the Advanced Light Source (ALS) synchrotron facility. The gratings were fabricated using a set of nanofabrication techniques including e-beam lithography, nanoimprint, plasma etch, and anisotropic wet etching. Two gratings with groove density of 6000 lines/mm and 3000 lines/mm and optimized for operation in the 1st and 2nd negative diffraction order respectively were fabricated and tested. We report on fabrication details and characterization of the gratings at beamline 6.3.2 of the ALS.

Highly efficient ultra-low blaze angle multilayer grating.

We have developed an advanced process for blaze angle reduction of x-ray gratings for the soft, tender, and EUV spectral ranges. The process is based on planarization of an anisotropically etched Si blazed grating followed by a chemically selective plasma etch. This provides a way to adjust the blaze angle to any lower value with high accuracy. Here we demonstrate the reduction of the blaze angle to an extremely low value of 0.04°±0.004°. For a 100 lines/mm grating with a Mo/Si multilayer coating, the grating exhibits diffraction efficiency of 58% in the 1st diffraction order at a wavelength of 13.3 nm. This technique will be applicable to a wide range of uses of high efficiency gratings for synchrotron sources, as well as for Free Electron Lasers (FEL).

Water-Window X-Ray Pulses from a Laser-Plasma Driven Undulator.

Femtosecond (fs) x-ray pulses are a key tool to study the structure and dynamics of matter on its natural length and time scale. To complement radio-frequency accelerator-based large-scale facilities, novel laser-based mechanisms hold promise for compact laboratory-scale x-ray sources. Laser-plasma driven undulator radiation in particular offers high peak-brightness, optically synchronized few-fs pulses reaching into the few-nanometer (nm) regime. To date, however, few experiments have successfully demonstrated plasma-driven undulator radiation. Those that have, typically operated at single and comparably long wavelengths. Here we demonstrate plasma-driven undulator radiation with octave-spanning tuneability at discrete wavelengths reaching from 13 nm to 4 nm. Studying spontaneous undulator radiation is an important step towards a plasma-driven free-electron laser. Our specific setup creates a photon pulse, which closely resembles the plasma electron bunch length and charge profile and thus might enable novel methods to characterize the longitudinal electron phase space.

Ultra-low blaze angle gratings for synchrotron and free electron laser applications.

We have developed a method for the manufacture of x-ray diffraction gratings with arbitrarily small blaze angles. These gratings are made by a process in which a high blaze angle grating made by anisotropic etching of Si (111) is subjected to planarization and reactive ion etching. Differential etching of the planarization medium and silicon ensures reduction of the blaze angle. Repeated application of this process leads to gratings of increasing perfection with an arbitrarily small blaze angle. This opens the way to highly efficient low line density gratings, to damage resistant gratings for ultra-high power applications such as free electron lasers, and for extension of the use of gratings into the hard x-ray energy range for dispersive spectroscopy.

Large area nanoimprint enables ultra-precise x-ray diffraction gratings.

A process for fabrication of ultra-precise diffraction gratings for high resolution x-ray spectroscopy was developed. A grating pattern with constant or variable line spacing (VLS) is recorded on a quartz plate by use of e-beam lithography with nanometer scale accuracy of the groove placement. The pattern is transferred to a massive grating blank by large area nanoimprint followed by dry or/and wet etching for groove shaping. High fidelity of the nanoimprint transfer step was confirmed by differential wavefront measurements. Successful implementation of the suggested fabrication approach was demonstrated by fabrication of a lamellar 900 lines/mm VLS grating for a soft x-ray fluorescence spectrometer.

Refraction effects in soft x-ray multilayer blazed gratings.

A 2500 lines/mm Multilayer Blazed Grating (MBG) optimized for the soft x-ray wavelength range was fabricated and tested. The grating coated with a W/B4C multilayer demonstrated a record diffraction efficiency in the 2nd blazed diffraction order in the energy range from 500 to 1200 eV. Detailed investigation of the diffraction properties of the grating demonstrated that the diffraction efficiency of high groove density MBGs is not limited by the normal shadowing effects that limits grazing incidence x-ray grating performance. Refraction effects inherent in asymmetrical Bragg diffraction were experimentally confirmed for MBGs. The refraction affects the blazing properties of the MBGs and results in a shift of the resonance wavelength of the gratings and broadening or narrowing of the grating bandwidth depending on diffraction geometry. The true blaze angle of the MBGs is defined by both the real structure of the multilayer stack and by asymmetrical refraction effects. Refraction effects can be used as a powerful tool in providing highly efficient suppression of high order harmonics.

Demonstration of the high collection efficiency of a broadband Mo/Si multilayer mirror with a graded multilayer coating on an ellipsoidal substrate.

A graded and broadband Mo/Si multilayer mirror for EUV spectroscopy is demonstrated. This mirror has an average reflectivity profile of 16% in the wavelength region from 15 nm to 17 nm and an effective area of 1100-1500 mm(2). This reflectivity is about 4 times larger than that of a standard Mo/Si multilayer mirror on a 1 in. diameter substrate, showing that the mirror can be used for measuring EUV fluorescence at wavelengths in the region around 15 nm to 17 nm.

Aqueous solution/metal interfaces investigated in operando by photoelectron spectroscopy.

We describe a new in operando approach for the investigation of heterogeneous processes at solid/liquid interfaces with elemental and chemical specificity which combines the preparation of thin liquid films using the meniscus method with standing wave ambient pressure X-ray photoelectron spectroscopy [Nemsák et al., Nat. Commun., 5, 5441 (2014)]. This technique provides information about the chemical composition across liquid/solid interfaces with sub-nanometer depth resolution and under realistic conditions of solution composition and concentration, pH, as well as electrical bias. In this article, we discuss the basics of the technique and present the first results of measurements on KOH/Ni interfaces.

Enhancement of diffraction efficiency via higher-order operation of a multilayer blazed grating.

Imperfections in the multilayer stack deposited on a saw-tooth substrate are the main factor limiting the diffraction efficiency of extreme ultraviolet and soft x-ray multilayer-coated blazed gratings (MBGs). Since the multilayer perturbations occur in the vicinity of antiblazed facets of the substrates, reduction of the groove density of MBGs is expected to enlarge the area of unperturbed multilayer and result in higher diffraction efficiency. At the same time the grating should be optimized for higher-order operation in order to keep high dispersion and spectral resolution. In this work we show the validity of this approach and demonstrate significant enhancement of diffraction efficiency of MBGs using higher-order diffraction. A new record for diffraction efficiency of 52% in the second diffraction order was achieved for an optimized MBG with groove density of 2525 lines/mm at the wavelength of 13.4 nm.

Ultra-high efficiency multilayer blazed gratings through deposition kinetic control.

Diffraction efficiency of multilayer-coated blazed gratings (MBG) strongly depends on the perfection of the sawtooth-shaped layers in the overall composite structure. Growth of multilayers on sawtooth substrates should be carefully optimized to reduce groove profile distortion and, at the same time, to avoid significant roughening of multilayer interfaces. In this work, we report on a way to optimize growth of sputter-deposited Mo/Si multilayers on sawtooth substrates through variation of the sputtering gas pressure. We believe a new record for diffraction efficiency of 44% was achieved for an optimized MBG with groove density of 5250 lines/mm at the wavelength of 13.1 nm.

Suppression of near-Fermi level electronic states at the interface in a LaNiO3/SrTiO3 superlattice.

Standing-wave-excited photoemission is used to study a SrTiO3/LaNiO3 superlattice. Rocking curves of core-level and valence band spectra are used to derive layer-resolved spectral functions, revealing a suppression of electronic states near the Fermi level in the multilayer as compared to bulk LaNiO3. Further analysis shows that the suppression of these states is not homogeneously distributed over the LaNiO3 layers but is more pronounced near the interfaces. Possible origins of this effect and its relationship to a previously observed metal-insulator-transition in ultrathin LaNiO3 films are discussed.

A 10,000 groove/mm multilayer coated grating for EUV spectroscopy.

Ultra-high spectral resolution in the EUV and soft x-ray energy ranges requires the use of very high line density gratings with optimal design resulting in use of a Blazed Multilayer Grating (BMG) structure. Here we demonstrate the production of near-atomically perfect Si blazed substrates with an ultra-high groove density (10,000 l/mm) together with the measured and theoretical performance of an Al/Zr multilayer coating on the grating. A 1st order absolute efficiency of 13% and 24.6% was achieved at incidence angles of 11° and 36° respectively. Cross-sectional TEM shows the effect of smoothing caused by the surface mobility of deposited atoms and we correlate this effect with a reduction in peak diffraction efficiency. This work shows the high performance that can be achieved with BMGs based on small-period anisotropic etched Si substrates, but also the constraints imposed by the surface mobility of deposited species.

Damage mechanisms of MoN/SiN multilayer optics for next-generation pulsed XUV light sources.

We investigated the damage mechanism of MoN/SiN multilayer XUV optics under two extreme conditions: thermal annealing and irradiation with single shot intense XUV pulses from the free-electron laser facility in Hamburg - FLASH. The damage was studied "post-mortem" by means of X-ray diffraction, interference-polarizing optical microscopy, atomic force microscopy, and scanning transmission electron microscopy. Although the timescale of the damage processes and the damage threshold temperatures were different (in the case of annealing it was the dissociation temperature of Mo2N and in the case of XUV irradiation it was the melting temperature of MoN) the main damage mechanism is very similar: molecular dissociation and the formation of N2, leading to bubbles inside the multilayer structure.

Single shot damage mechanism of Mo/Si multilayer optics under intense pulsed XUV-exposure.

We investigated single shot damage of Mo/Si multilayer coatings exposed to the intense fs XUV radiation at the Free-electron LASer facility in Hamburg - FLASH. The interaction process was studied in situ by XUV reflectometry, time resolved optical microscopy, and "post-mortem" by interference-polarizing optical microscopy (with Nomarski contrast), atomic force microscopy, and scanning transmission electron microcopy. An ultrafast molybdenum silicide formation due to enhanced atomic diffusion in melted silicon has been determined to be the key process in the damage mechanism. The influence of the energy diffusion on the damage process was estimated. The results are of significance for the design of multilayer optics for a new generation of pulsed (from atto- to nanosecond) XUV sources.

Tri-material multilayer coatings with high reflectivity and wide bandwidth for 25 to 50 nm extreme ultraviolet light.

Magnesium/silicon carbide (Mg/SiC) multilayers have been fabricated with normal incidence reflectivity in the vicinity of 40% to 50% for wavelengths in the 25 to 50 nm wavelength range. However many applications, for example solar telescopes and ultrafast studies using high harmonic generation sources, desire larger bandwidths than provided by high reflectivity Mg/SiC multilayers. We investigate introducing a third material, Scandium, to create a tri-material Mg/Sc/SiC multilayer allowing an increase the bandwidth while maintaining high reflectivity.

Single-cycle nonlinear optics.

Nonlinear optics plays a central role in the advancement of optical science and laser-based technologies. We report on the confinement of the nonlinear interaction of light with matter to a single wave cycle and demonstrate its utility for time-resolved and strong-field science. The electric field of 3.3-femtosecond, 0.72-micron laser pulses with a controlled and measured waveform ionizes atoms near the crests of the central wave cycle, with ionization being virtually switched off outside this interval. Isolated sub-100-attosecond pulses of extreme ultraviolet light (photon energy approximately 80 electron volts), containing approximately 0.5 nanojoule of energy, emerge from the interaction with a conversion efficiency of approximately 10(-6). These tools enable the study of the precision control of electron motion with light fields and electron-electron interactions with a resolution approaching the atomic unit of time ( approximately 24 attoseconds).

Experimental technique for radiative-process-resolved X-ray absorption spectroscopy at the inner-shell excitation thresholds.

Partial-fluorescence-yield (PFY) x-ray absorption measurements, rising the optimized window widths of position sensitive detectors in wave-length dispersive x-ray spectrometers, have been applied for radiative process-resolved (RPR) x-ray absorption spectroscopy. We have measured PFY-absorption spectra of graphite and diamond at the C K threshold and of h-BN and c-BN at the B K threshold. Resonant elastic x-ray scattering was observed in graphite and h-BN on their PFY-absorption spectra, and excitonic x-ray scattering was observed in diamond and c-BN. These results show that PFY-absorption measurements for RPR x-ray absorption spectroscopy can provide the information about the electronic structures and the radiative-decay process in inner-shell excitation.

Efficient high-order diffraction of extreme-ultraviolet light and soft x-rays by nanostructured volume gratings.

We report what is believed to be the first demonstration that volume gratings diffract extreme-ultraviolet light (EUV) or soft x-rays into high orders approximately an order of magnitude more efficiently than predicted by classical thin-grating theory. At the 13-nm wavelength, copolymer grating structures with 200-nm period and aspect ratios of ~10:1 achieved diffraction efficiencies of 11.2%, 15.3%, 11.5%, and 9.1% in the orders m of 2, 3, 4, and 5, respectively. In addition, the measured transmission spectra are consistent with electrodynamic calculations by coupled-wave theory. High-order diffraction can now be employed for substantially improved diffractive EUV and x-ray optics, e.g., highly resolving diffractive lenses and large-aperture condensers.

Transmission phase gratings for EUV interferometry.

The performance of the recently developed EUV phase-shifting point diffraction interferometer (PS/PDI) depends heavily on the characteristics of the grating beamsplitter used in the implementation. Ideally, such a grating should provide throughput of better than 25% and diffraction efficiency, defined as the ratio of the first-diffracted-order power to the zero-order power, variable in the range from approximately 10 to 500. The optimal method for achieving these goals is by way of a phase grating. Also, PS/PDI system implementation issues favor the use of transmission gratings over reflection gratings. Here, the design, fabrication, and characterization of a recently developed transmission phase grating developed for use in EUV interferometry is described.