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Molecular disordering of the ice surface occurs below the bulk meltingtemperature of 273 K, termed surface premelting. The top-most molecular layerbegins gradually premelting at 200 K, and has been linked to its lowcoefficient of friction through an increase in molecular mobility. The secondmolecular bilayer premelts around 257 K, but no study has linked thistransition to a change in any macroscopic phenomena. Here, we show that thethermodynamic work of adhesion between polydimethylsiloxane (PDMS) and icechanges abruptly at 257.0 $\pm$ 0.1 K. Surface-sensitive sum frequencygeneration spectroscopy shows that there are no molecular level changes at thePDMS surface or the ice-PDMS interface near the transition in adhesion,indicating that the transition arises from changes of the ice surface. Usingexisting contact angle data in the literature, we show that this transition isdue to a decrease in the acid-base component of the surface free energy of iceby 17 $\pm$ 2 mJ/m$^2$ at 257.0 $\pm$ 0.1 K. The change in surface energyprovides a possible explanation for a variety of unexplained phenomena seenacross the literature including ice adhesion, friction, and the morphology ofsnowflakes.

Transition in the Acid-Base Component of Surface Free Energy of Ice upon the Premelting of its Second Molecular Bilayer