Bulk and interfacial liquid water as a transient network

The special macroscopic properties of liquid water stem from its structure as a complex network of molecules connected by hydrogen bonds. While the dynamics of single molecules within this network has been extensively investigated, only little attention has been paid to the closed loops (meshes) of hydrogen-bonded molecules which determine the network topology. Using molecular dynamics simulations we analyze the size, shape, geometrical arrangement, and dynamical stability of loops containing up to 10 hydrogen bonds. We find that six-membered loops in liquid water even at room temperature retain a striking similarity with the well-known structure of ice. Analyzing the network dynamics we find that rings of more than five hydrogen bonds are stabilized compared to a random collection containing the same number of single bonds. We finally show that in the vicinity of hydrophobic and hydrophilic interfaces loops arrange in a preferred orientation.