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Author: Reimann, Klaus × DDC: 540 ×

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    A Mechanistic Perspective on Plastically Flexible Coordination Polymers
    (Weinheim : Wiley-VCH, 2019) Bhattacharya, Biswajit; Michalchuk, Adam A.L.; Silbernagl, Dorothee; Rautenberg, Max; Schmid, Thomas; Feiler, Torvid; Reimann, Klaus; Ghalgaoui, Ahmed; Sturm, Heinz; Paulus, Beate; Emmerling, Franziska
    Mechanical flexibility in single crystals of covalently bound materials is a fascinating and poorly understood phenomenon. We present here the first example of a plastically flexible one-dimensional (1D) coordination polymer. The compound [Zn(μ-Cl)2(3,5-dichloropyridine)2]n is flexible over two crystallographic faces. Remarkably, the single crystal remains intact when bent to 180°. A combination of microscopy, diffraction, and spectroscopic studies have been used to probe the structural response of the crystal lattice to mechanical bending. Deformation of the covalent polymer chains does not appear to be responsible for the observed macroscopic bending. Instead, our results suggest that mechanical bending occurs by displacement of the coordination polymer chains. Based on experimental and theoretical evidence, we propose a new model for mechanical flexibility in 1D coordination polymers. Moreover, our calculations propose a cause of the different mechanical properties of this compound and a structurally similar elastic material. © 2019 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.
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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.