Alexander Firsov

A novel monochromator for experiments with ultrashort X‐ray pulses

Aiming at advancing storage-ring-based ultrafast X-ray science, over the past few years many upgrades have been undertaken to continue improving beamline performance and photon flux at the Femtoslicing facility at BESSY II. In this article the particular design upgrade of one of the key optical components, the zone-plate monochromator (ZPM) beamline, is reported. The beamline is devoted to optical pump/soft X-ray probe applications with 100 fs (FWHM) X-ray pulses in the soft X-ray range at variable polarization. A novel approach consisting of an array of nine off-axis reflection zone plates is used for a gapless coverage of the spectral range between 410 and 1333 eV at a designed resolution of E/ΔE = 500 and a pulse elongation of only 30 fs. With the upgrade of the ZPM the following was achieved: a smaller focus, an improved spectral resolution and bandwidth as well as excellent long-term stability. The beamline will enable a new class of ultrafast applications with variable optical excitation wavelength and variable polarization.

Monochromatization of femtosecond XUV light pulses with the use of reflection zone plates.

We report on a newly built laser-based tabletop setup which enables generation of femtosecond light pulses in the XUV range employing the process of high-order harmonic generation (HHG) in a gas medium. The spatial, spectral, and temporal characteristics of the XUV beam are presented. Monochromatization of XUV light with minimum temporal pulse distortion is the central issue of this work. Off-center reflection zone plates are shown to be advantageous when selection of a desired harmonic is carried out with the use of a single optical element. A cross correlation technique was applied to characterize the performance of the zone plates in the time domain. By using laser pulses of 25 fs length to pump the HHG process, a pulse duration of 45 fs for monochromatized harmonics was achieved in the present setup.

X-ray absorption spectroscopy using a self-seeded soft X-ray free-electron laser

X-ray free electron lasers (XFELs) enable unprecedented new ways to study the electronic structure and dynamics of transition metal systems. L-edge absorption spectroscopy is a powerful technique for such studies and the feasibility of this method at XFELs for solutions and solids has been demonstrated. However, the required x-ray bandwidth is an order of magnitude narrower than that of self-amplified spontaneous emission (SASE), and additional monochromatization is needed. Here we compare L-edge x-ray absorption spectroscopy (XAS) of a prototypical transition metal system based on monochromatizing the SASE radiation of the linac coherent light source (LCLS) with a new technique based on self-seeding of LCLS. We demonstrate how L-edge XAS can be performed using the self-seeding scheme without the need of an additional beam line monochromator. We show how the spectral shape and pulse energy depend on the undulator setup and how this affects the x-ray spectroscopy measurements.

New Developments in Femtosecond Soft X‐ray Spectroscopy

Recent instrumentation developments in X‐ray spectroscopy for ultra‐fast time‐resolved measurements with soft X‐rays done in HZB Berlin during the last years are described. The significant performance improvements achieved this way are based on Fresnel diffraction from structures being fabricated on a surface of a total externally reflecting mirror. The first type of this spectrometer, an off‐axis reflection zone plate, has been implemented at the BESSY Femtoslicing setup and shows on the order of 20 times higher flux in the focal plane compared to the classical grating monochromator beamline. It has proven to serve very precise experiments with a time resolution down to 100 fs on magnetic materials after optical laser pulse excitation.

Design and optimization of a parallel spectrometer for ultra-fast X-ray science.

In the present work, different varied line space (VLS) and reflection zone plate (RZP) gratings are analyzed for their suitability in low-signal femtosecond soft X-ray spectroscopy. The need for high efficiency suggests a straightened focal line whose sharpness and residual curvature will determine the quality. One- and two-dimensional VLS structures feature an attractive trade-off between a sufficient optical performance and a strongly relaxed fabrication, due to moderate line densities which are easily accessible by e-beam lithography. Based on fanned-out RZP arrays, their continuous limit version is identified to generate an almost perfect focal line however, with an aberration level three orders of magnitude better than for the VLS gratings and well below the diffraction limit over large acceptance angles.

Graded crystal monochromator at Bessy II

The first successful tests of a graded crystal x-ray monochromator at BESSY II based on SiGe crystals are reported. The monochromator crystals with Ge concentration gradient of 0.8%/cm along the crystal surface have been tested at the KMC- 2 beamline. The beam from the BESSY II bending magnet with vertical divergence of 0.2 mrad was used. In comparison with conventional Si crystals the enhancement of an energy resolution is 3 - 5 times and, simultaneously, increase of spectral flux density of 4 - 6 times were obtained.

Femtosecond high-resolution hard X-ray spectroscopy using reflection zone plates.

An off-axis total external reflection zone plate is applied to wavelength-dispersive X-ray spectrometry in the range from 7.8 keV to 9.0 keV. The resolving power E/ΔE of up to 1.1 × 10(2), demonstrated in a synchrotron proof-of-concept experiment, competes well with existing energy-dispersive instruments in this spectral range. In conjunction with the detection efficiency of (2.2 ± 0.6)%, providing a fairly constant count rate across the 1.2 keV band, the temporal pulse elongation to no more than 1.5 × 10(-15) s opens the door to wide-range, ultra-fast hard X-ray spectroscopy at free-electron lasers (FELs).

Monochromatizing and focussing femtosecond high-order harmonic radiation with one optical element.

A novel approach for monochromatizing and focussing the Vacuum-Ultraviolet and soft x-ray radiation from high-order harmonic generation of a femtosecond optical laser with only one optical element is presented. We demonstrate that off-axis reflection zone plates applied as focussing monochromators allow for efficiently optimizing the trade-off between energy resolution and temporal dispersion of the femtosecond pulses. In the current experimental realization, we show how the temporal dispersion can be varied between 2 fs and 16 fs with a correlating variation of the energy resolution E/ΔE between 20 and 90 for an off-axis reflection zone plate optimized for harmonic 13 at 20.41 eV. We also show how the focal spot size varies correspondingly between 80 × 90 μm(2) and 290 × 140 μm(2) as determined with a computational fitting approach based on a 3D Gaussian model. The diffraction efficiency for the tested zone plates amounts to up to 10%. We furthermore evaluate the influence of pointing stability on the performance of the zone plates. Based on our results we propose an optimized realization of a dedicated beam line for femtosecond pulses from high-order harmonic generation with an off-axis reflection zone plate.

Reflection zone plate wavelength-dispersive spectrometer for ultra-light elements measurements.

We have developed an electron beam excitation ultra-soft X-ray add-on device for a scanning electron microscope with a reflective zone plate mulichannel spectrometer in order to analyse ultra-light elements such as Li and B. This spectrometer has high (λ/Δλ~100) resolving power in the energy range of 45 eV - 1120 eV. Metallic Li samples were examined and fluorescence spectra successfully measured. Energy resolution of 0.49 eV was measured in the ultra-low energy range using the Al L(2,3) line at 71 eV. High sensitivity of Boron detection was demonstrated on a B(4)C sample with layer thicknesses of 1-50 nm, detecting an amount of metallic Boron as small as ~0.57 fg.

New parallel wavelength-dispersive spectrometer based on scanning electron microscope

A new wavelength - dispersive X-ray spectrometer for scanning electron microscopy (SEM) has been developed. This spectrometer can cover an energy range from 50 eV to 1120 eV by using an array made of seventeen reflection zone plates. Soft X-ray emission spectra of simple elements of Li, Be, B, C, N, Ti, V, O, Cr, Mn, Fe, Co, Ni, Cu, Zn and Ga were measured. The overall energy resolving power on the order of E/ΔE ~80 to 160 has been demonstrated. Spectrometer with 200 reflection zone plates has been used as a multi-channel analyser in the energy range of 100 - 1000 eV for quasi - continuous spectra measurements. The predicted energy-resolving power on the order of E/ΔE = 50 has been achieved in the entire energy range.