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Surface freezing is a phenomenon in which crystallization is enhanced at avapor-liquid interface. In some systems, such as $n$-alkanes, this enhancementis dramatic, and results in the formation of a crystalline layer at the freeinterface even at temperatures slightly above the equilibrium bulk freezingtemperature. There are, however, systems in which the enhancement is purelykinetic, and only involves faster nucleation at or near the interface. Thefirst, thermodynamic, type of surface freezing is easier to confirm inexperiments, requiring only the verification of the existence of crystallineorder at the interface. The second, kinetic, type of surface freezing is farmore difficult to prove experimentally. One material that is suspected ofundergoing the second type of surface freezing is liquid water. Despite strongindications that the freezing of liquid water is kinetically enhanced atvapor-liquid interfaces, the findings are far from conclusive, and the topicremains controversial. In this perspective, we present a simple thermodynamicframework to understand conceptually and distinguish these two types of surfacefreezing. We then briefly survey fifteen years of experimental andcomputational work aimed at elucidating the surface freezing conundrum inwater.

Perspective: Surface Freezing in Water: A Nexus of Experiments and Simulations