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Because it is sensitive to fluctuations occurring over femtoseconds topicoseconds, gigahertz-to-terahertz dielectric relaxation spectroscopy canprovide a valuable window into water's most rapid intermolecular motions. Inresponse, we have built a vector network analyzer dielectric spectrometercapable of measuring absorbance and index of refraction in this frequencyregime with unprecedented precision. Using this to determine the complexdielectric response of water and aqueous salt solutions from 5.9 GHz to 1.12THz (which we provide in the SI), we have obtained strong new constraints ontheories of water's collective dynamics. For example, while thesalt-dependencies we observe for water's two slower relaxations (8 and 1 ps)are easily reconciled with suggestions that they arise due to rotations offully and partially hydrogen bonded molecules, respectively, thesalt-dependence of the fastest relaxation (180 fs) appears difficult toreconcile with its prior assignment to liberations of single hydrogen bonds.

High-precision gigahertz-to-terahertz spectroscopy of aqueous salt solutions as a probe of the femtosecond-to-picosecond dynamics of liquid water