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- ItemIn situ single-shot diffractive fluence mapping for X-ray free-electron laser pulses([London] : Nature Publishing Group UK, 2018) Schneider, Michael; Günther, Christian M.; Pfau, Bastian; Capotondi, Flavio; Manfredda, Michele; Zangrando, Marco; Mahne, Nicola; Raimondi, Lorenzo; Pedersoli, Emanuele; Naumenko, Denys; Eisebitt, StefanFree-electron lasers (FELs) in the extreme ultraviolet (XUV) and X-ray regime opened up the possibility for experiments at high power densities, in particular allowing for fluence-dependent absorption and scattering experiments to reveal non-linear light-matter interactions at ever shorter wavelengths. Findings of such non-linear effects are met with tremendous interest, but prove difficult to understand and model due to the inherent shot-to-shot fluctuations in photon intensity and the often structured, non-Gaussian spatial intensity profile of a focused FEL beam. Presently, the focused beam is characterized and optimized separately from the actual experiment. Here, we present the simultaneous measurement of XUV diffraction signals from solid samples in tandem with the corresponding single-shot spatial fluence distribution on the actual sample. Our in situ characterization scheme enables direct monitoring of the sample illumination, providing a basis to optimize and quantitatively understand FEL experiments.
- ItemReference shape effects on Fourier transform holography(Washington, DC : Soc., 2022) Malm, Erik; Pfau, Bastian; Schneider, Michael; Günther, Christian M.; Hessing, Piet; Büttner, Felix; Mikkelsen, Anders; Eisebitt, StefanSoft-x-ray holography which utilizes an optics mask fabricated in direct contact with the sample, is a widely applied x-ray microscopy method, in particular, for investigating magnetic samples. The optics mask splits the x-ray beam into a reference wave and a wave to illuminate the sample. The reconstruction quality in such a Fourier-transform holography experiment depends primarily on the characteristics of the reference wave, typically emerging from a small, high-aspect-ratio pinhole in the mask. In this paper, we study two commonly used reference geometries and investigate how their 3D structure affects the reconstruction within an x-ray Fourier holography experiment. Insight into these effects is obtained by imaging the exit waves from reference pinholes via high-resolution coherent diffraction imaging combined with three-dimensional multislice simulations of the x-ray propagation through the reference pinhole. The results were used to simulate Fourier-transform holography experiments to determine the spatial resolution and precise location of the reconstruction plane for different reference geometries. Based on our findings, we discuss the properties of the reference pinholes with view on application in soft-x-ray holography experiments.
- ItemUltrafast Demagnetization Dominates Fluence Dependence of Magnetic Scattering at Co M Edges(College Park, Md. : APS, 2020) Schneider, Michael; Pfau, Bastian; Günther, Christian M.; von Korff Schmising, Clemens; Weder, David; Geilhufe, Jan; Perron, Jonathan; Capotondi, Flavio; Pedersoli, Emanuele; Manfredda, Michele; Hennecke, Martin; Vodungbo, Boris; Lüning, Jan; Eisebitt, StefanWe systematically study the fluence dependence of the resonant scattering cross-section from magnetic domains in Co/Pd-based multilayers. Samples are probed with single extreme ultraviolet (XUV) pulses of femtosecond duration tuned to the Co M3,2 absorption resonances using the FERMI@Elettra free-electron laser. We report quantitative data over 3 orders of magnitude in fluence, covering 16 mJ/cm2/pulse to 10 000 mJ/cm2/pulse with pulse lengths of 70 fs and 120 fs. A progressive quenching of the diffraction cross-section with fluence is observed. Compression of the same pulse energy into a shorter pulse—implying an increased XUV peak electric field—results in a reduced quenching of the resonant diffraction at the Co M3,2 edge. We conclude that the quenching effect observed for resonant scattering involving the short-lived Co 3p core vacancies is noncoherent in nature. This finding is in contrast to previous reports investigating resonant scattering involving the longer-lived Co 2p states, where stimulated emission has been found to be important. A phenomenological model based on XUV-induced ultrafast demagnetization is able to reproduce our entire set of experimental data and is found to be consistent with independent magneto-optical measurements of the demagnetization dynamics on the same samples.
- ItemSingleshot polychromatic coherent diffractive imaging with a high-order harmonic source(Washington, DC : Soc., 2020) Malm, Erik; Wikmark, Hampus; Pfau, Bastian; Villanueva-Perez, Pablo; Rudawski, Piotr; Peschel, Jasper; Maclot, Sylvain; Schneider, Michael; Eisebitt, Stefan; Mikkelsen, Anders; L’Huillier, Anne; Johnsson, PerSingleshot polychromatic coherent diffractive imaging is performed with a high-intensity high-order harmonic generation source. The coherence properties are analyzed and several reconstructions show the shot-to-shot fluctuations of the incident beam wavefront. The method is based on a multi-step approach. First, the spectrum is extracted from double-slit diffraction data. The spectrum is used as input to extract the monochromatic sample diffraction pattern, then phase retrieval is performed on the quasi-monochromatic data to obtain the sample’s exit surface wave. Reconstructions based on guided error reduction (ER) and alternating direction method of multipliers (ADMM) are compared. ADMM allows additional penalty terms to be included in the cost functional to promote sparsity within the reconstruction. © 2020 Optical Society of America under the terms of the OSA Open Access Publishing Agreement.
- ItemAchieving diffraction-limited resolution in soft-X-ray Fourier-transform holography(Amsterdam : Elsevier Science, 2020) Geilhufe, Jan; Pfau, Bastian; Günther, Christian M.; Schneider, Michael; Eisebitt, StefanThe spatial resolution of microscopic images acquired via X-ray Fourier-transform holography is limited by the source size of the reference wave and by the numerical aperture of the detector. We analyze the interplay between both influences and show how they are matched in practice. We further identify, how high spatial frequencies translate to imaging artifacts in holographic reconstructions where mainly the reference beam limits the spatial resolution. As a solution, three methods are introduced based on numerical post-processing of the reconstruction. The methods comprise apodization of the hologram, refocusing via wave propagation, and deconvolution using the transfer function of the imaging system. In particular for the latter two, we demonstrate that image details smaller than the source size of the reference beam can be recovered up to the diffraction limit of the hologram. Our findings motivate the intentional application of a large reference-wave source enhancing the image contrast in applications with low photon numbers such as single-shot experiments at free-electron lasers or imaging at laboratory sources.
- ItemReal-time spatial characterization of micrometer-sized X-ray free-electron laser beams focused by bendable mirrors(Washington, DC : Soc., 2022) Mercurio, Giuseppe; Chalupský, Jaromír; Nistea, Ioana-Theodora; Schneider, Michael; Hájková, Věra; Gerasimova, Natalia; Carley, Robert; Cascella, Michele; Le Guyader, Loïc; Mercadier, Laurent; Schlappa, Justine; Setoodehnia, Kiana; Teichmann, Martin; Yaroslavtsev, Alexander; Burian, Tomáš; Vozda, Vojtĕch; Vyšín, Luděk; Wild, Jan; Hickin, David; Silenzi, Alessandro; Stupar, Marijan; Torben Delitz, Jan; Broers, Carsten; Reich, Alexander; Pfau, Bastian; Eisebitt, Stefan; La Civita, Daniele; Sinn, Harald; Vannoni, Maurizio; Alcock, Simon G.; Juha, Libor; Scherz, AndreasA real-time and accurate characterization of the X-ray beam size is essential to enable a large variety of different experiments at free-electron laser facilities. Typically, ablative imprints are employed to determine shape and size of μm-focused X-ray beams. The high accuracy of this state-of-the-art method comes at the expense of the time required to perform an ex-situ image analysis. In contrast, diffraction at a curved grating with suitably varying period and orientation forms a magnified image of the X-ray beam, which can be recorded by a 2D pixelated detector providing beam size and pointing jitter in real time. In this manuscript, we compare results obtained with both techniques, address their advantages and limitations, and demonstrate their excellent agreement. We present an extensive characterization of the FEL beam focused to ≈1 μm by two Kirkpatrick-Baez (KB) mirrors, along with optical metrology slope profiles demonstrating their exceptionally high quality. This work provides a systematic and comprehensive study of the accuracy provided by curved gratings in real-time imaging of X-ray beams at a free-electron laser facility. It is applied here to soft X-rays and can be extended to the hard X-ray range. Furthermore, curved gratings, in combination with a suitable detector, can provide spatial properties of μm-focused X-ray beams at MHz repetition rate.
- ItemGenerating circularly polarized radiation in the extreme ultraviolet spectral range at the free-electron laser FLASH(Melville, NY : American Institute of Physics, 2017) von Korff Schmising, Clemens; Weder, David; Noll, Tino; Pfau, Bastian; Hennecke, Martin; Strüber, Christian; Radu, Ilie; Schneider, Michael; Staeck, Steffen; Günther, Christian M.; Lüning, Jan; Merhe, Alaa el dine; Buck, Jens; Hartmann, Gregor; Viefhaus, Jens; Treusch, Rolf; Eisebitt, StefanA new device for polarization control at the free electron laser facility FLASH1 at DESY has been commissioned for user operation. The polarizer is based on phase retardation upon reflection off metallic mirrors. Its performance is characterized in three independent measurements and confirms the theoretical predictions of efficient and broadband generation of circularly polarized radiation in the extreme ultraviolet spectral range from 35 eV to 90 eV. The degree of circular polarization reaches up to 90% while maintaining high total transmission values exceeding 30%. The simple design of the device allows straightforward alignment for user operation and rapid switching between left and right circularly polarized radiation.
- ItemExperimental evaluation of signal-to-noise in spectro-holography via modified uniformly redundant arrays in the soft x-ray and extreme ultraviolet spectral regime(Bristol : IOP Publ., 2017-05-08) Günther, Christian M.; Guehrs, Erik; Schneider, Michael; Pfau, Bastian; von Korff Schmising, Clemens; Geilhufe, Jan; Schaffert, Stefan; Eisebitt, StefanWe present dichroic x-ray lensless magnetic imaging by Fourier transform holography with an extended reference scheme via a modified uniformly redundant array (mURA). Holographic images of magnetic domains simultaneously generated by a single pinhole reference as well as by a mURA reference are compared with respect to the signal-to-noise ratio (SNR) as a function of exposure time. We apply this approach for spectro-holographic imaging of ferromagnetic domain patterns in Co/Pt multilayer films. Soft x-rays with wavelengths of 1.59 nm (Co L3 absorption edge) and 20.8 nm (Co M2,3 absorption edges) are used for image formation and to generate contrast via x-ray magnetic circular dichroism. For a given exposure time, the mURA-based holography allows to decouple the reconstruction SNR from the spatial resolution. For 1.59 nm wavelength, the reconstruction via the extended reference scheme shows no significant loss of spatial resolution compared to the single pinhole reference. In contrast, at 20.8 nm wavelength the single pinhole reveals some very intricate features which are lost in the image generated by the mURA, although overall a high-quality image is generated. The SNR-advantage of the mURA scheme is most notable when the hologram has to be encoded with few photons, while errors associated with the increased complexity of the reconstruction process reduce the advantage for high-photon-number experiments.
- ItemCoherent correlation imaging for resolving fluctuating states of matter(London : Macmillan Publishers Limited, 2023) Klose, Christopher; Büttner, Felix; Hu, Wen; Mazzoli, Claudio; Litzius, Kai; Battistelli, Riccardo; Lemesh, Ivan; Bartell, Jason M.; Huang, Mantao; Günther, Christian M.; Schneider, Michael; Barbour, Andi; Wilkins, Stuart B.; Beach, Geoffrey S. D.; Eisebitt, Stefan; Pfau, BastianFluctuations and stochastic transitions are ubiquitous in nanometre-scale systems, especially in the presence of disorder. However, their direct observation has so far been impeded by a seemingly fundamental, signal-limited compromise between spatial and temporal resolution. Here we develop coherent correlation imaging (CCI) to overcome this dilemma. Our method begins by classifying recorded camera frames in Fourier space. Contrast and spatial resolution emerge by averaging selectively over same-state frames. Temporal resolution down to the acquisition time of a single frame arises independently from an exceptionally low misclassification rate, which we achieve by combining a correlation-based similarity metric1,2 with a modified, iterative hierarchical clustering algorithm3,4. We apply CCI to study previously inaccessible magnetic fluctuations in a highly degenerate magnetic stripe domain state with nanometre-scale resolution. We uncover an intricate network of transitions between more than 30 discrete states. Our spatiotemporal data enable us to reconstruct the pinning energy landscape and to thereby explain the dynamics observed on a microscopic level. CCI massively expands the potential of emerging high-coherence X-ray sources and paves the way for addressing large fundamental questions such as the contribution of pinning5–8 and topology9–12 in phase transitions and the role of spin and charge order fluctuations in high-temperature superconductivity13,14.
- ItemMulti-color imaging of magnetic Co/Pt heterostructures(Melville, NY : AIP Publishing LLC, 2017) Willems, Felix; von Korff Schmising, Clemens; Weder, David; Günther, Christian M.; Schneider, Michael; Pfau, Bastian; Meise, Sven; Guehrs, Erik; Geilhufe, Jan; Merhe, Alaa El Din; Jal, Emmanuelle; Vodungbo, Boris; Lüning, Jan; Mahieu, Benoit; Capotondi, Flavio; Pedersoli, Emanuele; Gauthier, David; Manfredda, Michele; Eisebitt, StefanWe present an element specific and spatially resolved view of magnetic domainsin Co/Pt heterostructures in the extreme ultraviolet spectral range. Resonantsmall-angle scattering and coherent imaging with Fourier-transform holographyreveal nanoscale magnetic domain networks via magnetic dichroism of Co at theM2,3 edges as well as via strong dichroic signals at the O2,3 and N6,7 edges of Pt.We demonstrate for the first time simultaneous, two-color coherent imaging at afree-electron laser facility paving the way for a direct real space access toultrafast magnetization dynamics in complex multicomponent material systems.