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Author: Ghalgaoui, Ahmed × DDC: 530 ×

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    Field-Induced Tunneling Ionization and Terahertz-Driven Electron Dynamics in Liquid Water
    (Washington, DC : ACS, 2020) Ghalgaoui, Ahmed; Koll, Lisa-Marie; Schütte, Bernd; Fingerhut, Benjamin P.; Reimann, Klaus; Woerner, Michael; Elsaesser, Thomas
    Liquid water at ambient temperature displays ultrafast molecular motions and concomitant fluctuations of very strong electric fields originating from the dipolar H2O molecules. We show that such random intermolecular fields induce the tunnel ionization of water molecules, which becomes irreversible if an external terahertz (THz) pulse imposes an additional directed electric field on the liquid. Time-resolved nonlinear THz spectroscopy maps charge separation, transport, and localization of the released electrons on a few-picosecond time scale. The highly polarizable localized electrons modify the THz absorption spectrum and refractive index of water, a manifestation of a highly nonlinear response. Our results demonstrate how the interplay of local electric field fluctuations and external electric fields allows for steering charge dynamics and dielectric properties in aqueous systems. Copyright © 2020 American Chemical Society.
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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.