Molecular polarizability anisotropy of liquid water revealed by terahertz-induced transient orientation

Nature Communications
Peter ZaldenChristian Bressler

Abstract

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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Citations

Apr 8, 2020·Physical Chemistry Chemical Physics : PCCP·Hossam Elgabarty, Thomas D Kühne
Aug 17, 2018·Physical Review. E·Hermann Grabert, Michael Thorwart
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Jan 16, 2021·Optics Letters·Hang ZhaoLiangliang Zhang
Feb 16, 2021·The Journal of Physical Chemistry. B·Viktor F Rozsa, Giulia Galli
Apr 4, 2021·The Journal of Chemical Physics·Klaus ReimannThomas Elsaesser
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Dec 20, 2019·The Journal of Physical Chemistry Letters·Zhi ZhuBo Song
Sep 28, 2021·Physical Chemistry Chemical Physics : PCCP·Fabio NovelliMartina Havenith

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