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Now showing 1 - 8 of 8
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    Linear chirped slope profile for spatial calibration in slope measuring deflectometry
    (Melville, NY : American Institute of Physics, 2016) Siewert, F.; Zeschke, T.; Arnold, T.; Paetzelt, H; Yashchuk, V.V.
    Slope measuring deflectometry is commonly used by the X-ray optics community to measure the long-spatial-wavelength surface figure error of optical components dedicated to guide and focus X-rays under grazing incidence condition at synchrotron and free electron laser beamlines. The best performing instruments of this kind are capable of absolute accuracy on the level of 30-50 nrad. However, the exact bandwidth of the measurements, determined at the higher spatial frequencies by the instrument’s spatial resolution, or more generally by the instrument’s modulation transfer function (MTF) is hard to determine. An MTF calibration method based on application of a test surface with a one-dimensional (1D) chirped height profile of constant amplitude was suggested in the past. In this work, we propose a new approach to designing the test surfaces with a 2D-chirped topography, specially optimized for MTF characterization of slope measuring instruments. The design of the developed MTF test samples based on the proposed linear chirped slope profiles (LCSPs) is free of the major drawback of the 1D chirped height profiles, where in the slope domain, the amplitude strongly increases with the local spatial frequency of the profile. We provide the details of fabrication of the LCSP samples. The results of first application of the developed test samples to measure the spatial resolution of the BESSY-NOM at different experimental arrangements are also presented and discussed.
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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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    A transportable Paul-trap for levitation and accurate positioning of micron-scale particles in vacuum for laser-plasma experiments
    (Melville, NY : American Institute of Physics, 2018) Ostermayr, T.M.; Gebhard, J.; Haffa, D.; Kiefer, D.; Kreuzer, C.; Allinger, K.; Bömer, C.; Braenzel, J.; Schnürer, M.; Cermak, I.; Schreiber, J.; Hilz, P.
    We report on a Paul-trap system with large access angles that allows positioning of fully isolated micrometer-scale particles with micrometer precision as targets in high-intensity laser-plasma interactions. This paper summarizes theoretical and experimental concepts of the apparatus as well as supporting measurements that were performed for the trapping process of single particles.
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    On the role of non-diagonal system-environment interactions in bridge-mediated electron transfer
    (Melville, NY : American Institute of Physics, 2020) Acharyya, Nirmalendu; Ovcharenko, Roman; Fingerhut, Benjamin P.
    Bridge-mediated electron transfer (ET) between a donor and an acceptor is prototypical for the description of numerous most important ET scenarios. While multi-step ET and the interplay of sequential and direct superexchange transfer pathways in the donor-bridge-acceptor (D-B-A) model are increasingly understood, the influence of off-diagonal system-bath interactions on the transfer dynamics is less explored. Off-diagonal interactions account for the dependence of the ET coupling elements on nuclear coordinates (non-Condon effects) and are typically neglected. Here, we numerically investigate with quasi-adiabatic propagator path integral simulations the impact of off-diagonal system-environment interactions on the transfer dynamics for a wide range of scenarios in the D-B-A model. We demonstrate that off-diagonal system-environment interactions can have profound impact on the bridge-mediated ET dynamics. In the considered scenarios, the dynamics itself does not allow for a rigorous assignment of the underlying transfer mechanism. Furthermore, we demonstrate how off-diagonal system-environment interaction mediates anomalous localization by preventing long-time depopulation of the bridge B and how coherent transfer dynamics between donor D and acceptor A can be facilitated. The arising non-exponential short-time dynamics and coherent oscillations are interpreted within an equivalent Hamiltonian representation of a primary reaction coordinate model that reveals how the complex vibronic interplay of vibrational and electronic degrees of freedom underlying the non-Condon effects can impose donor-to-acceptor coherence transfer on short timescales. © 2020 Author(s).
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    Ultrafast phosphate hydration dynamics in bulk H2O
    (Melville, NY : American Institute of Physics, 2015) Costard, Rene; Tyborski, Tobias; Fingerhut, Benjamin P.; Elsaesser, Thomas
    Phosphate vibrations serve as local probes of hydrogen bonding and structural fluctuations of hydration shells around ions. Interactions of H2PO4− ions and their aqueous environment are studied combining femtosecond 2D infrared spectroscopy, ab-initio calculations, and hybrid quantum-classical molecular dynamics (MD) simulations. Two-dimensional infrared spectra of the symmetric (𝜈𝑆(PO−2)) and asymmetric (𝜈𝐴𝑆(PO−2)) PO−2 stretching vibrations display nearly homogeneous lineshapes and pronounced anharmonic couplings between the two modes and with the δ(P-(OH)2) bending modes. The frequency-time correlation function derived from the 2D spectra consists of a predominant 50 fs decay and a weak constant component accounting for a residual inhomogeneous broadening. MD simulations show that the fluctuating electric field of the aqueous environment induces strong fluctuations of the 𝜈𝑆(PO−2) and 𝜈𝐴𝑆(PO−2) transition frequencies with larger frequency excursions for 𝜈𝐴𝑆(PO−2). The calculated frequency-time correlation function is in good agreement with the experiment. The 𝜈(PO−2) frequencies are mainly determined by polarization contributions induced by electrostatic phosphate-water interactions. H2PO4−/H2O cluster calculations reveal substantial frequency shifts and mode mixing with increasing hydration. Predicted phosphate-water hydrogen bond (HB) lifetimes have values on the order of 10 ps, substantially longer than water-water HB lifetimes. The ultrafast phosphate-water interactions observed here are in marked contrast to hydration dynamics of phospholipids where a quasi-static inhomogeneous broadening of phosphate vibrations suggests minor structural fluctuations of interfacial water.
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    Two-color two-dimensional terahertz spectroscopy: A new approach for exploring even-order nonlinearities in the nonperturbative regime
    (Melville, NY : American Institute of Physics, 2021) Woerner, Michael; Ghalgaoui, Ahmed; Reimann, Klaus; Elsaesser, Thomas
    Nonlinear two-dimensional terahertz (2D-THz) spectroscopy at frequencies of the emitted THz signal different from the driving frequencies allows for exploring the regime of (off-)resonant even-order nonlinearities in condensed matter. To demonstrate the potential of this method, we study two phenomena in the nonlinear THz response of bulk GaAs: (i) The nonlinear THz response to a pair of femtosecond near-infrared pulses unravels novel fourth- and sixth-order contributions involving interband shift currents, Raman-like excitations of transverse-optical phonon and intervalence-band coherences. (ii) Transient interband tunneling of electrons driven by ultrashort mid-infrared pulses can be effectively controlled by a low-frequency THz field with amplitudes below 50 kV/cm. The THz field controls the electron–hole separation modifying decoherence and the irreversibility of carrier generation.
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    Vibrational sum-frequency generation spectroscopy of lipid bilayers at repetition rates up to 100 kHz
    (Melville, NY : American Institute of Physics, 2018) Yesudas, Freeda; Mero, Mark; Kneipp, Janina; Heiner, Zsuzsanna
    Broadband vibrational sum-frequency generation (BB-VSFG) spectroscopy has become a well-established surface analytical tool capable of identifying the orientation and structure of molecular layers. A straightforward way to boost the sensitivity of the technique could be to increase the laser repetition rate beyond that of standard BB-VSFG spectrometers, which rely on Ti:sapphire lasers operating at repetition rates of 1-5 kHz. Nevertheless, possible thermally induced artifacts in the vibrational spectra due to higher laser average powers are unexplored. Here, we discuss laser power induced temperature accumulation effects that distort the BB-VSFG spectra of 1,2-diacyl-sn-glycero-3-phosphocholine at an interface between two transparent phases at repetition rates of 5, 10, 50, and 100 kHz at constant pulse energy. No heat-induced distortions were found in the spectra, suggesting that the increase in the laser repetition rate provides a feasible route to an improved signal-to-noise ratio or shorter data acquisition times in BB-VSFG spectroscopy for thin films on transparent substrates. The results have implications for future BB-VSFG spectrometers pushing the detection limit for molecular layers with low surface coverage.
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    Percolation of rigid fractal carbon black aggregates
    (Melville, NY : American Institute of Physics, 2021) Coupette, Fabian; Zhang, Long; Kuttich, Björn; Chumakov, Andrei; Roth, Stephan V.; González-García, Lola; Kraus, Tobias; Schilling, Tanja
    We examine network formation and percolation of carbon black by means of Monte Carlo simulations and experiments. In the simulation, we model carbon black by rigid aggregates of impenetrable spheres, which we obtain by diffusion-limited aggregation. To determine the input parameters for the simulation, we experimentally characterize the micro-structure and size distribution of carbon black aggregates. We then simulate suspensions of aggregates and determine the percolation threshold as a function of the aggregate size distribution. We observe a quasi-universal relation between the percolation threshold and a weighted average radius of gyration of the aggregate ensemble. Higher order moments of the size distribution do not have an effect on the percolation threshold. We conclude further that the concentration of large carbon black aggregates has a stronger influence on the percolation threshold than the concentration of small aggregates. In the experiment, we disperse the carbon black in a polymer matrix and measure the conductivity of the composite. We successfully test the hypotheses drawn from simulation by comparing composites prepared with the same type of carbon black before and after ball milling, i.e., on changing only the distribution of aggregate sizes in the composites.