title: Competing coexisting phases in 2D water.
abstract: The properties of bulk water come from a delicate balance of interactions on length scales encompassing several orders of magnitudes: i) the Hydrogen Bond (HBond) at the molecular scale and ii) the extension of this HBond network up to the macroscopic level. Here, we address the physics of water when the three dimensional extension of the HBond network is frustrated, so that the water molecules are forced to organize in only two dimensions. We account for the large scale fluctuating HBond network by an analytical mean-field percolation model. This approach provides a coherent interpretation of the different events experimentally (calorimetry, neutron, NMR, near and far infra-red spectroscopies) detected in interfacial water at 160, 220 and 250 K. Starting from an amorphous state of water at low temperature, these transitions are respectively interpreted as the onset of creation of transient low density patches of 4-HBonded molecules at 160 K, the percolation of these domains at 220 K and finally the total invasion of the surface by them at 250 K. The source of this surprising behaviour in 2D is the frustration of the natural bulk tetrahedral local geometry and the underlying very significant increase in entropy of the interfacial water molecules.
authors.affiliation: Laboratoire Léon Brillouin, CEA, CNRS, Université Paris-Saclay, CEA Saclay, 91191 Gif-sur-Yvette Cedex, France.
authors.forename: Jean-Marc
authors.initials: JM
authors.lastname: Zanotti
authors.affiliation: Laboratoire Léon Brillouin, CEA, CNRS, Université Paris-Saclay, CEA Saclay, 91191 Gif-sur-Yvette Cedex, France.|ICMMO, (UMR CNRS 8182), Univ. Paris-Sud, Université Paris-Saclay, 91405 Orsay, France.
authors.forename: Patrick
authors.initials: P
authors.lastname: Judeinstein
authors.affiliation: Synchrotron SOLEIL, L'Orme des Merisiers, BP 48, Gif-sur-Yvette Cedex F-91192, France.
authors.forename: Simona
authors.initials: S
authors.lastname: Dalla-Bernardina
authors.affiliation: Synchrotron SOLEIL, L'Orme des Merisiers, BP 48, Gif-sur-Yvette Cedex F-91192, France.
authors.forename: Gaëlle
authors.initials: G
authors.lastname: Creff
authors.affiliation: Synchrotron SOLEIL, L'Orme des Merisiers, BP 48, Gif-sur-Yvette Cedex F-91192, France.
authors.forename: Jean-Blaise
authors.initials: JB
authors.lastname: Brubach
authors.affiliation: Synchrotron SOLEIL, L'Orme des Merisiers, BP 48, Gif-sur-Yvette Cedex F-91192, France.
authors.forename: Pascale
authors.initials: P
authors.lastname: Roy
authors.affiliation: SPEC, CEA, CNRS, Université Paris-Saclay, CEA Saclay, 91191 Gif-sur-Yvette Cedex, France.
authors.forename: Marco
authors.initials: M
authors.lastname: Bonetti
authors.affiliation: Institut Laue Langevin, 38042 Grenoble CEDEX, France.
authors.forename: Jacques
authors.initials: J
authors.lastname: Ollivier
authors.affiliation: NIMBE, CEA, CNRS, Université Paris-Saclay, CEA Saclay, 91191 Gif-sur-Yvette Cedex, France.
authors.forename: Dimitrios
authors.initials: D
authors.lastname: Sakellariou
authors.affiliation: Laboratoire Léon Brillouin, CEA, CNRS, Université Paris-Saclay, CEA Saclay, 91191 Gif-sur-Yvette Cedex, France.
authors.forename: Marie-Claire
authors.initials: MC
authors.lastname: Bellissent-Funel