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The liquid and supercooled states of water show a series of anomalies whosenature is debated. A key role is attributed to the formation of structuralaggregates induced by critical phenomena occurring deep in the supercooledregion; the nature of the water anomalies and of the hidden critical processesremains elusive. Here we report a time-resolved optical Kerr effectinvestigation of the vibrational dynamics and relaxation processes insupercooled bulk water. The experiment measures the water intermolecularvibrations and the structural relaxation process in an extended temperaturerange, and with unprecedented data quality. A mode-coupling analysis of theexperimental data enables to characterize the intermolecular vibrational modesand their interplay with the structural relaxation process. The results bringevidence of the coexistence of two local configurations, which are interpretedas high-density and low-density water forms, with an increasing weight of thelatter at low temperatures.

Evidence of two distinct local structures of water from ambient to supercooled conditions