Optimization of Cr/Sc-based multilayer mirrors for water window soft x-rays.

The development of efficient multilayer mirrors for the water window (a spectral region between absorption edges of carbon and oxygen, from 284 to 543 eV) remains a challenge. As the best candidate, the Cr/Sc multilayer provides maximum theoretical reflectivity of about 60% at near-normal incidence around the Sc L2,3 absorption edge (397 eV). However, the maximum measured peak reflectance published so far just slightly exceeds 20%. We report on a new (to the best of our knowledge) approach to design more efficient Cr/Sc-based multilayer coatings using the process of nitridation of chromium during deposition and adding boron carbide as a third material in the multilayer structure. We discuss our strategy of optimization of the CrN/B4C/Sc multilayer system based on experimental studies. The peak reflectance as high as 32% at 396 eV was measured with this type of coating, which is of main interest for various water window applications such as x-ray microscopy.

Experimental study and modeling of extreme ultraviolet 4000 lines/mm diffraction gratings coated with periodic and aperiodic Al/Mo/SiC multilayers.

Multilayer coated diffraction gratings are crucial components for extreme ultraviolet (EUV) applications such as spectroscopy or spectro-imaging. However, for high groove density, the smoothening of the grating surface profile with multilayer deposition remains a limitation that requires further investigation. In this paper, we report on the design, characterization, and modeling of 4000 lines/mm diffraction gratings coated with periodic and aperiodic Al/Mo/SiC multilayers for EUV radiation. Two types of gratings with different groove depths are compared. Multilayer coatings were designed using a genetic algorithm to maximize the first-order diffraction efficiency in the 17-21 and 19-23 nm wavelength ranges at normal incidence. Periodic and aperiodic multilayers with different numbers of layers were deposited by magnetron sputtering on the two types of fused silica gratings, and the grating groove profile evolution was measured by atomic force microscopy and cross-section transmission electron microscopy. The first-order diffraction efficiency was measured in the EUV at 5° incidence using monochromatic synchrotron radiation and modeled using the rigorous coupled-wave analysis method. The simulation models refined by using the Debye-Waller factor to account for the multilayer interfacial roughness show good agreement with experimental data. The results reported in this study will allow for designing efficient EUV multilayer gratings for high-resolution spectro-imaging instruments.

New method for the determination of photoabsorption from transmittance measurements in the extreme ultraviolet.

We have developed a new method for the determination of photoabsorption at extreme ultraviolet wavelengths longer than 20 nm, where reliable refractive index values are sparse or non-existent. Our method overcomes the obstacle of multiple reflections that occur inside thin films in this spectral range, which up until now has prevented the accurate determination of photoabsorption from transmittance measurements. We have derived a mathematical expression that is independent of internal reflection amplitudes, while taking advantage of the transmittance oscillations stemming from such reflections. The method is validated on measurements of aluminum thin films. This advance will enable accurate refractive index values for many important materials for optical instrumentation, thus facilitating high-priority research on topics including coherent light sources, planetary and solar physics, and semiconductor manufacturing.

Al/Mo/SiC multilayer diffraction gratings with broadband efficiency in the extreme ultraviolet.

Al/Mo/SiC periodic and aperiodic multilayers were optimized and deposited on high groove density gratings to achieve broadband efficiency in the extreme ultraviolet (EUV). Grating efficiencies were measured by monochromatic synchrotron radiation under 5° and 45° incident angles in the wavelength ranges 17-25 nm and 22-31 nm, respectively. We study the influence of the number of deposited periods on the initial trapezoidal profile and the EUV diffraction efficiency. We propose models of periodic and aperiodic coatings based on a combination of characterizations and compare rigorous coupled-wave analysis (RCWA) simulations with experimental data. We demonstrate the possibility to select the optimal balance between peak efficiency and bandwidth by adjusting the number of periods in the case of periodic multilayer grating. We also report unprecedented broadband diffraction efficiency with an Al/Mo/SiC aperiodic multilayer grating.

High efficiency Al/Sc-based multilayer coatings in the EUV wavelength range above 40 nanometers.

In this Letter, we have developed new and highly efficient periodic multilayer mirrors Al/Sc, Al/Sc/SiC, and Mo/Al/Sc with optimized reflectance at wavelengths between 40 and 65 nm. We have reached record values in measured peak reflectance: 57.5% at 44.7 nm and 46.5% at 51 nm, with Al/Sc/SiC at near-normal incidence. Furthermore, to the best of our knowledge, we have achieved the largest reported bandwidth with Mo/Al/Sc at 57 nm and the narrowest bandwidth with Al/Sc at a 60 nm wavelength. These new and promising results demonstrate that Al/Sc-based multilayer coatings are excellent candidates for future generations of extreme ultraviolet (EUV) instruments for solar physics, EUV lasers, and attosecond science, in a wavelength range that has not been fully explored.

Lifetime Stability and Microstructure Properties of Cr/B4C X-ray Reflective Multilayer Coatings.

This paper demonstrates that highly reflective Cr/B4C multilayer interference coatings with nanometric layer thicknesses, designed to operate in the soft X-ray photon energy range, have stable reflective performance for a period of 3 years after deposition. The microstructure and chemical composition of layers and interfaces within Cr/B4C multilayers is also examined, with emphasis on the B4C-on-Cr interface where a significant diffusion layer is formed and on the oxide in the top B4C layer. Multiple characterization techniques (X-ray reflectivity at different photon energies, X-ray photoelectron spectroscopy, transmission electron microscopy, electron diffraction and X-ray diffraction) are employed and the results reveal a consistent picture of the Cr/B4C layer structure.

Kossel Effect in Periodic Multilayers.

The Kossel effect is the diffraction by a periodically structured medium, of the characteristic X-ray radiation emitted by the atoms of the medium. We show that multilayers designed for X-ray optics applications are convenient periodic systems to use in order to produce the Kossel effect, modulating the intensity emitted by the sample in a narrow angular range defined by the Bragg angle. We also show that excitation can be done by using photons (X-rays), electrons or protons (or charged particles), under near normal or grazing incident geometries, which makes the method relatively easy to implement. The main constraint comes from the angular resolution necessary for the detection of the emitted radiation. This leads to small solid angles of detection and long acquisition times to collect data with sufficient statistical significance. Provided this difficulty is overcome, the comparison or fit of the experimental Kossel curves, i.e., the angular distributions of the intensity of an emitted radiation of one of the element of the periodic stack, with the simulated curves enables getting information on the depth distribution of the elements throughout the multilayer. Thus the same kind of information obtained from the more widespread method of X-ray standing wave induced fluorescence used to characterize stacks of nanometer period, can be obtained using the Kossel effect.

Phase measurement of soft x-ray multilayer mirrors.

We propose a new model enabling the extraction of the phase of a multilayer mirror from photocurrent measurements in the soft x rays. In this range, the effects of the mean free path of the electrons inside the stack can no longer be neglected, which prevents the phase reconstruction by conventional photocurrent measurements. The new model takes into account this phenomenon and thus extends up to the x rays the applicability range of the technique. This approach has been validated through a numerical and experimental study of chromium/scandium multilayers used near 360 eV. To our knowledge, this work constitutes the first measurement of the phase of a multilayer mirror in the soft x-ray range.

High-efficiency B4C/Mo2C alternate multilayer grating for monochromators in the photon energy range from 0.7 to 3.4 keV.

An alternate multilayer (AML) grating has been prepared by coating an ion etched lamellar grating with a B4C/Mo2C multilayer (ML) having a layer thickness close to the groove depth. Such a structure behaves as a 2D synthetic crystal and can reach very high efficiencies when the Bragg condition is satisfied. This AML coated grating has been characterized at the SOLEIL Metrology and Tests Beamline between 0.7 and 1.7 keV and at the four-crystal monochromator beamline of Physikalisch-Technische Bundesanstalt (PTB) at BESSY II between 1.75 and 3.4 keV. A peak diffraction efficiency of nearly 27% was measured at 2.2 keV. The measured efficiencies are well reproduced by numerical simulations made with the electromagnetic propagation code CARPEM. Such AML gratings, paired with a matched ML mirror, constitute efficient monochromators for intermediate energy photons. They will extend the accessible energy for many applications as x-ray absorption spectroscopy or x-ray magnetic circular dichroism experiments.

Polarization control of high order harmonics in the EUV photon energy range.

We report the generation of circularly polarized high order harmonics in the extreme ultraviolet range (18-27 nm) from a linearly polarized infrared laser (40 fs, 0.25 TW) focused into a neon filled gas cell. To circularly polarize the initially linearly polarized harmonics we have implemented a four-reflector phase-shifter. Fully circularly polarized radiation has been obtained with an efficiency of a few percents, thus being significantly more efficient than currently demonstrated direct generation of elliptically polarized harmonics. This demonstration opens up new experimental capabilities based on high order harmonics, for example, in biology and materials science. The inherent femtosecond time resolution of high order harmonic generating table top laser sources renders these an ideal tool for the investigation of ultrafast magnetization dynamics now that the magnetic circular dichroism at the absorption M-edges of transition metals can be exploited.

Structural properties of Al/Mo/SiC multilayers with high reflectivity for extreme ultraviolet light.

We present the results of an optical and chemical, depth and surface study of Al/Mo/SiC periodic multilayers, designed as high reflectivity coatings for the extreme ultra-violet (EUV) range. In comparison to the previously studied Al/SiC system, the introduction of Mo as a third material in the multilayer structure allows us to decrease In comparison to the previously studied Al/SiC system with a reflectance of 37% at near normal incidence around 17 nm, the introduction of Mo as a third material in the multilayer structure allows us to decrease the interfacial roughness and achieve an EUV reflectivity of 53.4%, measured with synchrotron radiation. This is the first report of a reflectivity higher than 50% around 17 nm. Time-of-flight secondary ion mass spectrometry (ToF-SIMS) and x-ray photoelectron spectroscopy (XPS) measurements are performed on the Al/Mo/SiC system in order to analyze the individual layers within the stack. ToF-SIMS and XPS results give evidence that the first SiC layer is partially oxidized, but the O atoms do not reach the first Mo and Al layers. We use these results to properly describe the multilayer stack and discuss the possible reasons for the difference between the measured and simulated EUV reflectivity values.

Spatiotemporal distortions of attosecond pulses.

In this article, we report that usual multilayer mirror configurations to focus attosecond pulses generate geometric aberrations and can significantly stretch pulses. The numerical simulations show that the effects can be strong enough to delay some parts of the pulses of an attosecond pulse train and make them interfere with the next pulses of the train. The influence of the numerical aperture on the pulse duration is also studied, showing that such effects can occur even with very low numerical apertures.

Design and characterization of extreme-ultraviolet broadband mirrors for attosecond science.

A novel multilayer mirror was designed and fabricated based on a recently developed three-material technology aimed both at reaching reflectivities of about 20% and at controlling dispersion over a bandwidth covering photon energies between 35 and 50 eV. The spectral phase upon reflection was retrieved by measuring interferences in a two-color ionization process using high-order harmonics produced from a titanium: sapphire laser. We demonstrate the feasibility of designing and characterizing phase-controlled broadband optics in the extreme-ultraviolet domain, which should facilitate the manipulation of attosecond pulses for applications.

Study of normal incidence of three-component multilayer mirrors in the range 20-40 nm.

We study theoretically and experimentally the increase of normal incidence reflectivity generated by addition of a third material in the period of a standard periodic multilayer, for wavelengths in the range 20 to 40 nm. The nature and thickness of the three materials has been optimized to provide the best enhancement of reflectivity. Theoretical reflectivity of an optimized B4C/Mo/Si multilayer reaches 42% at 32 nm. B4C/Mo/Si multilayers have been deposited with a magnetron sputtering system and a reflectivity of 34% at 32 nm has been measured on a synchrotron radiation source.

X-ray-ultraviolet beam splitters for the Michelson interferometer.

With the aim of realizing a Michelson interferometer working at 13.9 nm, we have developed a symmetrical beam splitter with multilayers deposited on the front and back sides of a silicon nitride membrane. On the basis of the experimental optical properties of the membrane, simulations have been performed to define the multilayer structure that provides the highest reflectivity-transmission product. Optimized Mo-Si multilayers have been successfully deposited on both sides of t he membrane by use of the ion-beam sputtering technique, with a thickness-period reproducibility of 0.1 nm. Measurements by means of synchrotron radiation at 13.9 nm and at an angle of 45 degrees provide a reflectivity of 14.2% and a transmission of 15.2% for a 60% s-polarized light, close to the simulated values. Such a beam splitter has been used for x-ray laser Michelson interferometry at 13.9 nm. The first interferogram is discussed.

Longitudinal coherence measurements of a transient collisional x-ray laser.

We present what is to our knowledge the first longitudinal coherence measurement of a transient inversion collisional x-ray laser. We investigated the picosecond output of a Ni-like Pd x-ray laser at 14.68 nm generated by the COMET laser facility at the Lawrence Livermore National Laboratory. Interference fringes were generated with a Michelson interferometer setup in which a thin multilayer membrane was used as a beam splitter. We determined the longitudinal coherence for the 4d1S0 --> 4p1P1 lasing transition to be approximately 400 microm (1/e half-width) by changing the length of one interferometer arm and measuring the resultant variation in fringe visibility. The inferred gain-narrowed linewidth of approximately 0.29 pm is a factor of 4 less than previously measured in quasi-steady-state x-ray laser schemes.