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    CAMP@FLASH: an end-station for imaging, electron- and ion-spectroscopy, and pump–probe experiments at the FLASH free-electron laser
    (Chester : IUCr, 2018-8-2) Erk, Benjamin; Müller, Jan P.; Bomme, Cédric; Boll, Rebecca; Brenner, Günter; Chapman, Henry N.; Correa, Jonathan; Düsterer, Stefan; Dziarzhytski, Siarhei; Eisebitt, Stefan; Graafsma, Heinz; Grunewald, Sören; Gumprecht, Lars; Hartmann, Robert; Hauser, Günter; Keitel, Barbara; von Korff Schmising, Clemens; Kuhlmann, Marion; Manschwetus, Bastian; Mercadier, Laurent; Müller, Erland; Passow, Christopher; Plönjes, Elke; Ramm, Daniel; Rompotis, Dimitrios; Rudenko, Artem; Rupp, Daniela; Sauppe, Mario; Siewert, Frank; Schlosser, Dieter; Strüder, Lothar; Swiderski, Angad; Techert, Simone; Tiedtke, Kai; Tilp, Thomas; Treusch, Rolf; Schlichting, Ilme; Ullrich, Joachim; Moshammer, Robert; Möller, Thomas; Rolles, Daniel
    The non-monochromatic beamline BL1 at the FLASH free-electron laser facility at DESY was upgraded with new transport and focusing optics, and a new permanent end-station, CAMP, was installed. This multi-purpose instrument is optimized for electron- and ion-spectroscopy, imaging and pump–probe experiments at free-electron lasers. It can be equipped with various electron- and ion-spectrometers, along with large-area single-photon-counting pnCCD X-ray detectors, thus enabling a wide range of experiments from atomic, molecular, and cluster physics to material and energy science, chemistry and biology. Here, an overview of the layout, the beam transport and focusing capabilities, and the experimental possibilities of this new end-station are presented, as well as results from its commissioning.
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    Terahertz magnetic field enhancement in an asymmetric spiral metamaterial
    (Bristol : IOP Publ., 2018-10-25) Polley, Debanjan; Hagström, Nanna Zhou; Schmising, Clemens von Korff; Eisebitt, Stefan; Bonetti, Stefano
    We use finite element simulations in both the frequency and the time-domain to study the terahertz resonance characteristics of a metamaterial (MM) comprising a spiral connected to a straight arm. The MM acts as a RLC circuit whose resonance frequency can be precisely tuned by varying the characteristic geometrical parameters of the spiral: inner and outer radius, width and number of turns. We provide a simple analytical model that uses these geometrical parameters as input to give accurate estimates of the resonance frequency. Finite element simulations show that linearly polarized terahertz radiation efficiently couples to the MM thanks to the straight arm, inducing a current in the spiral, which in turn induces a resonant magnetic field enhancement at the center of the spiral. We observe a large (approximately 40 times) and uniform (over an area of ∼10 μm2) enhancement of the magnetic field for narrowband terahertz radiation with frequency matching the resonance frequency of the MM. When a broadband, single-cycle terahertz pulse propagates towards the MM, the peak magnetic field of the resulting band-passed waveform still maintains a six-fold enhancement compared to the peak impinging field. Using existing laser-based terahertz sources, our MM design allows to generate magnetic fields of the order of 2 T over a time scale of several picoseconds, enabling the investigation of nonlinear ultrafast spin dynamics in table-top experiments. Furthermore, our MM can be implemented to generate intense near-field narrowband, multi-cycle electromagnetic fields to study generic ultrafast resonant terahertz dynamics in condensed matter.
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    Quantification of silver nanoparticle uptake and distribution within individual human macrophages by FIB/SEM slice and view
    (London : Biomed Central, 2017-3-21) Guehrs, Erik; Schneider, Michael; Günther, Christian M.; Hessing, Piet; Heitz, Karen; Wittke, Doreen; López-Serrano Oliver, Ana; Jakubowski, Norbert; Plendl, Johanna; Eisebitt, Stefan; Haase, Andrea
    Background: Quantification of nanoparticle (NP) uptake in cells or tissues is very important for safety assessment. Often, electron microscopy based approaches are used for this purpose, which allow imaging at very high resolution. However, precise quantification of NP numbers in cells and tissues remains challenging. The aim of this study was to present a novel approach, that combines precise quantification of NPs in individual cells together with high resolution imaging of their intracellular distribution based on focused ion beam/ scanning electron microscopy (FIB/SEM) slice and view approaches. Results: We quantified cellular uptake of 75 nm diameter citrate stabilized silver NPs (Ag 75 Cit) into an individual human macrophage derived from monocytic THP-1 cells using a FIB/SEM slice and view approach. Cells were treated with 10 μg/ml for 24 h. We investigated a single cell and found in total 3138 ± 722 silver NPs inside this cell. Most of the silver NPs were located in large agglomerates, only a few were found in clusters of fewer than five NPs. Furthermore, we cross-checked our results by using inductively coupled plasma mass spectrometry and could confirm the FIB/SEM results. Conclusions: Our approach based on FIB/SEM slice and view is currently the only one that allows the quantification of the absolute dose of silver NPs in individual cells and at the same time to assess their intracellular distribution at high resolution. We therefore propose to use FIB/SEM slice and view to systematically analyse the cellular uptake of various NPs as a function of size, concentration and incubation time.
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    Experimental 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, Stefan
    We 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.
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    Author Correction: Ultrafast X-ray imaging of the light-induced phase transition in VO2 (Nature Physics, (2022), 10.1038/s41567-022-01848-w)
    (Basingstoke : Nature Publishing Group, 2023) Johnson, Allan S.; Perez-Salinas, Daniel; Siddiqui, Khalid M.; Kim, Sungwon; Choi, Sungwook; Volckaert, Klara; Majchrzak, Paulina E.; Ulstrup, Søren; Agarwal, Naman; Hallman, Kent; Haglund, Richard F.; Günther, Christian M.; Pfau, Bastian; Eisebitt, Stefan; Backes, Dirk; Maccherozzi, Francesco; Fitzpatrick, Ann; Dhesi, Sarnjeet S.; Gargiani, Pierluigi; Valvidares, Manuel; Artrith, Nongnuch; de Groot, Frank; Choi, Hyeongi; Jang, Dogeun; Katoch, Abhishek; Kwon, Soonnam; Park, Sang Han; Kim, Hyunjung; Wall, Simon E.
    In the version of this article initially published, the Acknowledgements was missing thanks from Soonnam Kwon for support from the National Research Foundation of Korea (NRF-2020R1A2C1007416). The error has been corrected in the HTML and PDF versions of the article.
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    In 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, Stefan
    Free-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.
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    Coherent 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, Bastian
    Fluctuations 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.
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    Generating 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, Stefan
    A 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.
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    Quantitative hyperspectral coherent diffractive imaging spectroscopy of a solid-state phase transition in vanadium dioxide
    (Washington, DC [u.a.] : Assoc., 2021) Johnson, Allan S.; Conesa, Jordi Valls; Vidas, Luciana; Perez-Salinas, Daniel; Günther, Christian M.; Pfau, Bastian; Hallman, Kent A.; Haglund, Richard F.; Eisebitt, Stefan; Wall, Simon
    Solid-state systems can host a variety of thermodynamic phases that can be controlled with magnetic fields, strain, or laser excitation. Many phases that are believed to exhibit exotic properties only exist on the nanoscale, coexisting with other phases that make them challenging to study, as measurements require both nanometer spatial resolution and spectroscopic information, which are not easily accessible with traditional x-ray spectromicroscopy techniques. Here, we use coherent diffractive imaging spectroscopy (CDIS) to acquire quantitative hyperspectral images of the prototypical quantum material vanadium oxide across the vanadium L2,3 and oxygen K x-ray absorption edges with nanometer-scale resolution. We extract the full complex refractive indices of the monoclinic insulating and rutile conducting phases of VO2 from a single sample and find no evidence for correlation-driven phase transitions. CDIS will enable quantitative full-field x-ray spectromicroscopy for studying phase separation in time-resolved experiments and other extreme sample environments where other methods cannot operate.
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    Multi-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, Stefan
    We 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.