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Formation of local molecular structures in liquid water is believed to havemarked effect on the bulk properties of water, however, resolving suchstructural motives in an experiment is challenging. This challenge might behandled if the relevant low-frequency structural motion of the liquid isdirectly driven with an intense electromagnetic pulse. Here, we resonantlyexcite diffusive reorientational motions in water with intense terahertz pulsesand measure the resulting transient optical birefringence. The observedresponse is shown to arise from a particular configuration, namely therestricted trans-lational motion of water molecules whose motions arepredominantly orthogonal to the dipole moment of the excited neighboring watermolecules. Accordingly, we estimate the strength of the anharmonic couplingbetween the rotational and the restricted translational degrees of freedom ofwater.

Anharmonic Coupling between Intermolecular Motions of Water Revealed by Terahertz Kerr Effect