Revealing the Frank–Evans “Iceberg” Structures within the Solvation Layer around Hydrophobic Solutes

[Image: see text] Using computer simulations, the structural properties of solvation water of three model hydrophobic molecules, methane and two fullerenes (C60 and C80), were studied. Systems were simulated at temperatures in the range of 250–298 K. By analyzing both the local ordering of the molecules of water in the solvation layers and the structure of hydrogen bond network, it is shown that in the solvation layer of hydrophobic molecules, ordered aggregates consisting of water molecules are formed. Even though it is difficult to define the exact structure of these aggregates, their existence alone is clearly noticeable. Moreover, these aggregates become more pronounced with the decrease of temperature. The existence of the ordered aggregates around the hydrophobic solutes complies with the concept of “icebergs” proposed by Frank and Evans.