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Significance Hydrophobic interactions and other solvent-mediated noncovalent interactions are decisive for the stability and functionality of biomolecular structures over an extended range of conditions. A molecular theory should explain characteristic temperature dependences and help in modeling biomolecular structures and functions. So far, there has been just one theory of hydrophobic interactions, the Pratt–Chandler (PC) theory. The PC theory has not been definitively tested because of lack of quantitative correspondence between systems convenient for theory, simulation, and experiment. The present work adapts simulation results to atomic-scale hard-core models of the PC theory. Surprisingly, from the perspective of the PC theory, these results show that atomic-scale hydrophobic interactions between hard-sphere solutes are attractive and endothermic, thereby identifying a target for improved theories.

Molecular-scale hydrophobic interactions between hard-sphere reference solutes are attractive and endothermic