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Nature communications v.9 no.1, 2018년, pp.2142 - 2142   SCI SCIE
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Molecular polarizability anisotropy of liquid water revealed by terahertz-induced transient orientation

Zalden, Peter (Centre for Ultrafast Imaging CUI, University of Hamburg, 22761, Hamburg, Germany. peter.zalden@xfel.eu ) ; Song, Liwei (European XFEL, Holzkoppel 4, 22869, Schenefeld, Germany. peter.zalden@xfel.eu ) ; Wu, Xiaojun (Center for Free-Electron Laser Science CFEL, Deutsches Elektronen-Synchrotron, 22607, Hamburg, Germany ) ; Huang, Haoyu (State Key Laboratory of High Field Laser Physics, Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, 201800, Shanghai, China ) ; Ahr, Frederike (Center for Free-Electron Laser Science CFEL, Deutsches Elektronen-Synchrotron, 22607, Hamburg, Germany ) ; Mücke, Oliver D. (School of Electronic and Information Engineering, Beihang University, 100191, Beijing, China ) ; Reichert, Joscha (Center for Free-Electron Laser Science CFEL, Deutsches Elektronen-Synchrotron, 22607, Hamburg, Germany ) ; Thorwart, Michael (Center for Free-Electron Laser Science CFEL, Deutsches Elektronen-Synchrotron, 22607, Hamburg, Germany ) ; Mishra, Pankaj Kr. (Centre for Ultrafast Imaging CUI, University of Hamburg, 22761, Hamburg, Germany ) ; Welsch, Ralph (Center for Free-Electron Laser Science CFEL, Deutsches Elektron ) ; Santra, Robin ; Kärtner, Franz X. ; Bressler, Christian ;

  • 초록  

    Reaction pathways of biochemical processes are influenced by the dissipative electrostatic interaction of the reagents with solvent water molecules. The simulation of these interactions requires a parametrization of the permanent and induced dipole moments. However, the underlying molecular polarizability of water and its dependence on ions are partially unknown. Here, we apply intense terahertz pulses to liquid water, whose oscillations match the timescale of orientational relaxation. Using a combination of terahertz pump / optical probe experiments, molecular dynamics simulations, and a Langevin dynamics model, we demonstrate a transient orientation of their dipole moments, not possible by optical excitation. The resulting birefringence reveals that the polarizability of water is lower along its dipole moment than the average value perpendicular to it. This anisotropy, also observed in heavy water and alcohols, increases with the concentration of sodium iodide dissolved in water. Our results enable a more accurate parametrization and a benchmarking of existing and future water models.


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