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Subject: Electric fields Γ— WGL Institute: MBI Γ—

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Now showing 1 - 4 of 4
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    Photoelectron holography in strong optical and dc electric fields
    (Bristol : Institute of Physics Publishing, 2014) Stodolna, A.; Huismans, Y.; RouzΓ©e, A.; LΓ©pine, F.; Vrakking, M.J.J.
    The application of velocity map imaging for the detection of photoelectrons resulting from atomic or molecular ionization allows the observation of interferometric, and in some cases holographic structures that contain detailed information on the target from which the photoelecrons are extracted. In this contribution we present three recent examples of the use of photoelectron velocity map imaging in experiments where atoms are exposed to strong optical and dc electric fields. We discuss (i) observations of the nodal structure of Stark states of hydrogen measured in a dc electric field, (ii) mid-infrared strong-field ionization of metastable Xe atoms and (iii) the reconstruction of helium electronic wavepackets in an attosecond pump-probe experiment. In each case, the interference between direct and indirect electron pathways, reminiscent of the reference and signal waves in holography, is seen to play an important role.
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    Ultrafast two-dimensional terahertz spectroscopy of elementary excitations in solids
    (Bristol : IOP, 2013) Woerner, M.; Kuehn, W.; Bowlan, P.; Reimann, K.; Elsaesser, T.
    Recent experimental progress has allowed for the implementation of nonlinear two-dimensional (2D) terahertz (THz) spectroscopy in the ultrafast time domain. We discuss the principles of this technique based on multiple phase-locked electric field transients interacting in a collinear geometry with a solid and the phase-resolved detection of the THz fields after interaction with the sample. To illustrate the potential of this new method, 2D correlation spectra of coupled intersubband-longitudinal optical phonon excitations in a double quantum well system and a study of ultrafast carrier dynamics in graphene are presented.
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    Molecular couplings and energy exchange between DNA and water mapped by femtosecond infrared spectroscopy of backbone vibrations
    (Melville, NY : AIP Publishing LLC, 2017) Liu, Yingliang; Guchhait, Biswajit; Siebert, Torsten; Fingerhut, Benjamin P.; Elsaesser, Thomas
    Molecular couplings between DNA and water together with the accompanying processes of energy exchange are mapped via the ultrafast response of DNA backbone vibrations after OH stretch excitation of the water shell. Native salmon testes DNA is studied in femtosecond pump-probe experiments under conditions of full hydration and at a reduced hydration level with two water layers around the double helix. Independent of their local hydration patterns, all backbone vibrations in the frequency range from 940 to 1120 cm-1 display a quasi-instantaneous reshaping of the spectral envelopes of their fundamental absorption bands upon excitation of the water shell. The subsequent reshaping kinetics encompass a one-picosecond component, reflecting the formation of a hot ground state of the water shell, and a slower contribution on a time scale of tens of picoseconds. Such results are benchmarked by measurements with resonant excitation of the backbone modes, resulting in distinctly different absorption changes. We assign the fast changes of DNA absorption after OH stretch excitation to structural changes in the water shell which couple to DNA through the local electric fields. The second slower process is attributed to a flow of excess energy from the water shell into DNA, establishing a common heated ground state in the molecular ensemble. This interpretation is supported by theoretical calculations of the electric fields exerted by the water shell at different temperatures.
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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 H2PO4βˆ’ 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 (πœˆπ‘†(POβˆ’2)) and asymmetric (πœˆπ΄π‘†(POβˆ’2)) POβˆ’2 stretching vibrations display nearly homogeneous lineshapes and pronounced anharmonic couplings between the two modes and with the Ξ΄(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 πœˆπ‘†(POβˆ’2) and πœˆπ΄π‘†(POβˆ’2) transition frequencies with larger frequency excursions for πœˆπ΄π‘†(POβˆ’2). The calculated frequency-time correlation function is in good agreement with the experiment. The 𝜈(POβˆ’2) frequencies are mainly determined by polarization contributions induced by electrostatic phosphate-water interactions. H2PO4βˆ’/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.