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Now showing 1 - 10 of 12
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    Ultrafast Structural Changes in Chiral Molecules Measured with Free-Electron Lasers
    (Bristol : IOP Publ., 2020) Schmidt, P.; Music, V.; Hartmann, G.; Boll, R.; Erk, B.; Bari, S.; Allum, F.; Baumann, T.M.; Brenner, G.; Brouard, M.; Burt, M.; Coffee, R.; Dörner, S.; Galler, A.; Grychtol, P.; Heathcote, D.; Inhester, L.; Kazemi, M.; Larsson, M.; Li, Z.; Lutmann, A.; Manschwetus, B.; Marder, L.; Mason, R.; Moeller, S.; Osipov, T.; Otto, H.; Passow, C.; Rolles, D.; Rupprecht, P.; Schubert, K.; Schwob, L.; Thomas, R.; Vallance, C.; Von Korff Schmising, C.; Wagner, R.; Walter, P.; Wolf, T.J.A.; Zhaunerchyk, V.; Meyer, M.; Ehresmann, A.; Knie, A.; Demekhin, P.V.; Ilchen, M.
    (X-ray) free-electron lasers are employed to site specifically interrogate atomic fragments during ultra-fast photolysis of chiral molecules via time-resolved photoelectron circular dichroism. © 2020 Institute of Physics Publishing. All rights reserved.
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    Tailoring the stoichiometry of C3N4 nanosheets under electron beam irradiation
    (Cambridge : RSC Publ., 2021) Mendes, Rafael G.; Ta, Huy Q.; Yang, Xiaoqin; Bachmatiuk, Alicja; Praus, Petr; Mamakhel, Aref; Iversen, Bo B.; Su, Ren; Gemming, Thomas; Rümmeli, Mark H.
    Two-dimensional polymeric graphitic carbon nitride (g-C3N4) is a low-cost material with versatile properties that can be enhanced by the introduction of dopant atoms and by changing the degree of polymerization/stoichiometry, which offers significant benefits for numerous applications. Herein, we investigate the stability of g-C3N4 under electron beam irradiation inside a transmission electron microscope operating at different electron acceleration voltages. Our findings indicate that the degradation of g-C3N4 occurs with N species preferentially removed over C species. However, the precise nitrogen group from which N is removed from g-C3N4 (C–N–C, [double bond, length as m-dash]NH or –NH2) is unclear. Moreover, the rate of degradation increases with decreasing electron acceleration voltage, suggesting that inelastic scattering events (radiolysis) dominate over elastic events (knock-on damage). The rate of degradation by removing N atoms is also sensitive to the current density. Hence, we demonstrate that both the electron acceleration voltage and the current density are parameters with which one can use to control the stoichiometry. Moreover, as N species were preferentially removed, the d-spacing of the carbon nitride structure increased. These findings provide a deeper understanding of g-C3N4.
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    Sub-15-fs X-ray pump and X-ray probe experiment for the study of ultrafast magnetization dynamics in ferromagnetic alloys
    (Washington, DC : Soc., 2021) Liu, Xuan; Merhe, Alaaeldine; Jal, Emmanuelle; Delaunay, Renaud; Jarrier, Romain; Chardonnet, Valentin; Hennes, Marcel; Chiuzbaian, Sorin G.; Légaré, Katherine; Hennecke, Martin; Radu, Ilie; Von Korff Schmising, Clemens; Grunewald, Særen; Kuhlmann, Marion; Lüning, Jan; Vodungbo, Boris
    In this paper, we present a new setup for the measurement of element-specific ultrafast magnetization dynamics in ferromagnetic thin films with a sub-15-fs time resolution. Our experiment relies on a split and delay approach which allows us to fully exploit the shortest X-rays pulses delivered by X-ray Free Electrons Lasers (close to the attosecond range), in an X-ray pump – X-ray probe geometry. The setup performance is demonstrated by measuring the ultrafast elemental response of Ni and Fe during demagnetization of ferromagnetic Ni and Ni80Fe20 (Permalloy) samples upon resonant excitation at the corresponding absorption edges. The transient demagnetization process is measured in both reflection and transmission geometry using, respectively, the transverse magneto-optical Kerr effect (T-MOKE) and the Faraday effect as probing mechanisms.
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    Bulk single crystals and physical properties of β-(AlxGa1-x)2O3(x = 0-0.35) grown by the Czochralski method
    (Melville, NY : American Inst. of Physics, 2023) Galazka, Zbigniew; Fiedler, Andreas; Popp, Andreas; Ganschow, Steffen; Kwasniewski, Albert; Seyidov, Palvan; Pietsch, Mike; Dittmar, Andrea; Anooz, Saud Bin; Irmscher, Klaus; Suendermann, Manuela; Klimm, Detlef; Chou, Ta-Shun; Rehm, Jana; Schroeder, Thomas; Bickermann, Matthias
    We have systematically studied the growth, by the Czochralski method, and basic physical properties of a 2 cm and 2 in. diameter bulk β-(AlxGa1-x)2O3 single crystal with [Al] = 0-35 mol. % in the melt in 5 mol. % steps. The segregation coefficient of Al in the Ga2O3 melt of 1.1-1.2 results in a higher Al content in the crystals than in the melt. The crystals were also co-doped with Si or Mg. [Al] = 30 mol. % in the melt (33-36 mol. % in the crystals) seems to be a limit for obtaining bulk single crystals of high structural quality suitable for homoepitaxy. The crystals were either semiconducting (no intentional co-dopants with [Al] = 0-30 mol. % and Si-doped with [Al] = 15-20 mol. %), degenerately semiconducting (Si-doped with [Al] ≤ 15 mol. %), or semi-insulating ([Al] ≥ 25 mol. % and/or Mg-doped). The full width at half maximum of the rocking curve was 30-50 arcsec. The crystals showed a linear but anisotropic decrease in all lattice constants and a linear increase in the optical bandgap (5.6 eV for [Al] = 30 mol. %). The room temperature electron mobility at similar free electron concentrations gradually decreases with [Al], presumably due to enhanced scattering at phonons as the result of a larger lattice distortion. In Si co-doped crystals, the scattering is enhanced by ionized impurities. Measured electron mobilities and bandgaps enabled to estimate the Baliga figure of merit for electronic devices.
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    Terahertz transient stimulated emission from doped silicon
    (Melville, NY : AIP Publishing, 2020) Pavlov, S.G.; Deßmann, N.; Pohl, A.; Zhukavin, R.K.; Klaassen, T.O.; Abrosimov, N.V.; Riemann, H.; Redlich, B.; Van Der Meer, A.F.G.; Ortega, J.-M.; Prazeres, R.; Orlova, E.E.; Muraviev, A.V.; Shastin, V.N.; Hübers, H.-W.
    Transient-type stimulated emission in the terahertz (THz) frequency range has been achieved from phosphorus doped silicon crystals under optical excitation by a few-picosecond-long pulses generated by the infrared free electron lasers FELIX and CLIO. The analysis of the lasing threshold and emission spectra indicates that the stimulated emission occurs due to combined population inversion based lasing and stimulated Raman scattering. Giant gain has been obtained in the optically pumped silicon due to large THz cross sections of intracenter impurity transitions and resonant intracenter electronic scattering. The transient-type emission is formed under conditions when the pump pulse intervals exceed significantly the photon lifetime in the laser resonator. © 2020 Author(s).
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    Finding the semantic similarity in single-particle diffraction images using self-supervised contrastive projection learning
    (London : Nature Publ. Group, 2023) Zimmermann, Julian; Beguet, Fabien; Guthruf, Daniel; Langbehn, Bruno; Rupp, Daniela
    Single-shot coherent diffraction imaging of isolated nanosized particles has seen remarkable success in recent years, yielding in-situ measurements with ultra-high spatial and temporal resolution. The progress of high-repetition-rate sources for intense X-ray pulses has further enabled recording datasets containing millions of diffraction images, which are needed for the structure determination of specimens with greater structural variety and dynamic experiments. The size of the datasets, however, represents a monumental problem for their analysis. Here, we present an automatized approach for finding semantic similarities in coherent diffraction images without relying on human expert labeling. By introducing the concept of projection learning, we extend self-supervised contrastive learning to the context of coherent diffraction imaging and achieve a dimensionality reduction producing semantically meaningful embeddings that align with physical intuition. The method yields substantial improvements compared to previous approaches, paving the way toward real-time and large-scale analysis of coherent diffraction experiments at X-ray free-electron lasers.
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    Attosecond investigation of extreme-ultraviolet multi-photon multi-electron ionization
    (Washington, DC : OSA, 2022) Kretschmar, M.; Hadjipittas, A.; Major, B.; Tümmler, J.; Will, I.; Nagy, T.; Vrakking, M. J. J.; Emmanouilidou, A.; Schütte, B.
    Multi-electron dynamics in atoms and molecules very often occur on sub- to few-femtosecond time scales. The available intensities of extreme-ultraviolet (XUV) attosecond pulses have previously allowed the time-resolved investigation of two-photon, two-electron interactions. Here we study double and triple ionization of argon atoms involving the absorption of up to five XUV photons using a pair of intense attosecond pulse trains (APTs). By varying the time delay between the two APTs with attosecond precision and the spatial overlap with nanometer precision, we obtain information on complex nonlinear multi-photon ionization pathways. Our experimental and numerical results show that Ar2+ is predominantly formed by a sequential two-photon process, whereas the delay dependence of the Ar3+ ion yield exhibits clear signatures of the involvement of a simultaneous two-photon absorption process. Our experiment suggests that it is possible to investigate multi-electron dynamics using attosecond pulses for both pumping and probing the dynamics.
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    Compact intense extreme-ultraviolet source
    (Washington, DC : OSA, 2021) Major, Balázs; Ghafur, Omair; Kovács, Katalin; Varjú, Katalin; Tosa, Valer; Vrakking, Marc J. J.; Schütte, B.
    High-intensity laser pulses covering the ultraviolet to terahertz spectral regions are nowadays routinely generated in a large number of laboratories. In contrast, intense extreme-ultraviolet (XUV) pulses have only been demonstrated using a small number of sources including free-electron laser facilities [1-3] and long high-harmonic generation (HHG) beamlines [4-9]. Here we demonstrate a concept for a compact intense XUV source based on HHG that is focused to an intensity of $2 \times 10^{14}$ W/cm$^2$, with a potential increase up to $10^{17}$ W/cm$^2$ in the future. Our approach uses tight focusing of the near-infrared (NIR) driving laser and minimizes the XUV virtual source size by generating harmonics several Rayleigh lengths away from the NIR focus. Accordingly, the XUV pulses can be refocused to a small beam waist radius of 600 nm, enabling the absorption of up to four XUV photons by a single Ar atom in a setup that fits on a modest (2 m) laser table. Our concept represents a straightforward approach for the generation of intense XUV pulses in many laboratories, providing novel opportunities for XUV strong-field and nonlinear optics experiments, for XUV-pump XUV-probe spectroscopy and for the coherent diffractive imaging of nanoscale structures.
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    Real-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, Andreas
    A 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.
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    THz streak camera performance for single-shot characterization of XUV pulses with complex temporal structures
    (Washington, DC : Soc., 2020) Oelze, Tim; Kulyk, Olena; Schütte, Bernd; Frühling, Ulrike; Klimešová, Eva; Jagielski, Bartholomäus; Dittrich, Laura; Drescher, Markus; Pan, Rui; Stojanovic, Nikola; Polovinkin, Vitaly; Khakurel, Krishna P.; Muehlig, Kerstin; Bermudez Macias, Ivette J.; Düsterer, Stefan; Faatz, Bart; Andreasson, Jakob; Wieland, Marek; Krikunova, Maria
    The THz-field-driven streak camera has proven to be a powerful diagnostic-technique that enables the shot-to-shot characterization of the duration and the arrival time jitter of free electron laser (FEL) pulses. Here we investigate the performance of three computational approaches capable to determine the duration of FEL pulses with complex temporal structures from single-shot measurements of up to three simultaneously recorded spectra. We use numerically simulated FEL pulses in order to validate the accuracy of the pulse length retrieval in average as well as in a single-shot mode. We discuss requirements for the THz field strength in order to achieve reliable results and compare our numerical study with the analysis of experimental data that were obtained at the FEL in Hamburg - FLASH. © 2020 Optical Society of America under the terms of the OSA Open Access Publishing Agreement