Low-Density Water Structure Observed in a Nanosegregated Cryoprotectant Solution at Low Temperatures from 285 to 238 K

The structure of liquid water is defined by its molecular association through hydrogen bonding. Two different structures have been proposed for liquid water at low temperatures: low-density liquid (LDL) and high-density liquid (HDL) water. Here, we demonstrate a platform that can be exploited to experimentally probe the structure of liquid water in equilibrium at temperatures down to 238 K. We make use of a cryoprotectant molecule, glycerol, that, when mixed with water, lowers the freezing temperature of the solution nonmonotonically with glycerol concentration. We use a combination of neutron diffraction measurements and computational modeling to examine the structure of water in glycerol–water liquid mixtures at low temperatures from 285 to 238 K. We confirm that the mixtures are nanosegregated into regions of glycerol-rich and water-rich clusters. We examine the water structure and reveal that, at the temperatures studied here, water forms a low-density water structure that is more tetrahedral than the structure at room temperature. We postulate that nanosegregation allows water to form a low-density structure that is protected by an extensive and encapsulating glycerol interface.