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Tracking the excitation of water molecules in the homogeneous liquid ischallenging due to the ultrafast dissipation of rotational excitation energythrough the hydrogen-bonded network. Here we demonstrate strong transientanisotropy of liquid water through librational excitation using single-colorpump-probe experiments at 12.3 THz. We deduce a third order response of chi^3exceeding previously reported values in the optical range by three orders ofmagnitude. Using a theory that replaces the nonlinear response with a materialresponse property amenable to molecular dynamics simulation, we show that therotationally damped motion of water molecules in the librational band isresonantly driven at this frequency, which could explain the enhancement of theanisotropy in the liquid by the external Terahertz field. By addition of salt(MgSO4), the hydration water is instead dominated by the local electric fieldof the ions, resulting in reduction of water molecules that can be dynamicallyperturbed by THz pulses.

Strong Anisotropy in Liquid Water upon Librational Excitation using Terahertz Laser Fields