Phase-resolved sum-frequency generation measurements combined with molecular dynamics simu- lations are employed to study the effect of temperature on the molecular arrangement of water on the basal face of ice. The topmost monolayer, interrogated through its nonhydrogen-bonded, free O-H stretch peak, exhibits a maximum in surface H-bond density around 200 K. This maximum results from two competing effects: above 200 K, thermal fluctuations cause the breaking of H bonds; below 200 K, the formation of bulklike crystalline interfacial structures leads to H-bond breaking. Knowledge of the surface structure of ice is critical for understanding reactions occurring on ice surfaces and ice nucleation.

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Publisher APS
Funder NWO
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Journal Phys. Rev. Lett.
Smit, W.J, Tang, F, Sanchez, M.A, Backus, E.H.G, Xu, Limei, Hasegawa, T, … Nagata, Y. (2017). Excess Hydrogen Bond at the Ice-Vapor Interface around 200 K. Phys.Rev.Lett., 119(Article number: 133003), 1–5. doi:10.1103/PhysRevLett.119.133003