Correlation between Macroscopic and Microscopic Relaxation Dynamics of Water: Evidence for Two Liquid Forms

Abstract: Water is vital for life, and without it biomolecules and cells cannot maintain their structures and functions. The remarkable properties of water originate from its ability to form hydrogen-bonding networks and dynamics, which the connectivity constantly alters because of the orientation rotation of individual water molecules. Experimental investigation of the dynamics of water, however, has proven challenging due to the strong absorption of water at terahertz frequencies. In response, by employing a high-precision terahertz spectrometer, we have measured and characterized the terahertz dielectric response of water from supercooled liquid to near the boiling point to explore the motions. The response reveals dynamic relaxation processes corresponding to the collective orientation, single-molecule rotation, and structural rearrangements resulting from breaking and reforming hydrogen bonds in water. We have observed the direct relationship between the macroscopic and microscopic relaxation dynamics of water, and the results have provided evidence of two liquid forms in water with different transition temperatures and thermal activation energies. The results reported here thus provide an unprecedented opportunity to directly test microscopic computational models of water dynamics.