Pentagons and Heptagons in the First Water Layer on Pt(111)

Nie, Shu; Feibelman, Peter J.; Bartelt, N. C.; Thürmer, Konrad

doi:10.1103/physrevlett.105.026102

Cited by 229 publications

(272 citation statements)

References 21 publications

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“…As reported by Kimmel et al (36) and confirmed by our previous STM work (31), water deposited at 135-150 K onto Pt(111) first forms a one-molecule-thin wetting layer (37)(38)(39)(40). Then, isolated 3D ice crystallites emerge and eventually, at thicknesses of ∼3-10 nm, coalesce into a continuous multilayer film.…”

Section: Resultssupporting

confidence: 55%

Formation of hexagonal and cubic ice during low-temperature growth

Thürmer

Nie

2013

Proc. Natl. Acad. Sci. U.S.A.

109

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From our daily life we are familiar with hexagonal ice, but at very low temperature ice can exist in a different structure--that of cubic ice. Seeking to unravel the enigmatic relationship between these two low-pressure phases, we examined their formation on a Pt (111) substrate at low temperatures with scanning tunneling microscopy and atomic force microscopy. After completion of the onemolecule-thick wetting layer, 3D clusters of hexagonal ice grow via layer nucleation. The coalescence of these clusters creates a rich scenario of domain-boundary and screw-dislocation formation. We discovered that during subsequent growth, domain boundaries are replaced by growth spirals around screw dislocations, and that the nature of these spirals determines whether ice adopts the cubic or the hexagonal structure. Initially, most of these spirals are single, i.e., they host a screw dislocation with a Burgers vector connecting neighboring molecular planes, and produce cubic ice. Films thicker than ∼20 nm, however, are dominated by double spirals. Their abundance is surprising because they require a Burgers vector spanning two molecular-layer spacings, distorting the crystal lattice to a larger extent. We propose that these double spirals grow at the expense of the initially more common single spirals for an energetic reason: they produce hexagonal ice.ice growth mechanisms | molecular surface steps | molecular-layer nucleation | scanning probe microscopy | spiral growth O wing to its ubiquity in nature, ice and its structural properties have inspired widespread interest (1, 2). Not long after the introduction of X-ray diffraction in 1912, the structure of the most common modification of ice, hexagonal ice Ih, had already been investigated extensively (1-6). In 1942, König (7) discovered that at low temperatures water occasionally crystallizes into a different modification, cubic ice Ic. Subsequently, cubic ice has been produced in the laboratory, e.g., by condensing water vapor onto cooled substrates (7-11), by heating amorphous solid water (7-9), by supercooling liquid water droplets (12-14) or clusters (15), or by freezing high-pressure phases of ice and reheating them at atmospheric pressure (16)(17)(18)(19). Cubic ice has been proposed to also occur naturally, e.g., in the earth's atmosphere (13,(20)(21)(22)(23)(24) and in comets (25,26). However, even after thousands of articles dedicated to ice formation have appeared, important questions regarding fundamental growth mechanisms of ice remain. Some of these questions concerning the competition between the two lowpressure crystalline phases ice Ih and ice Ic are addressed in this paper.Ice Ih and ice Ic have been observed to coexist at temperatures up to 240 K (10-12, 18, 27, 28). When ice Ic is heated above 170 K it transforms irreversibly into ice Ih. The release of a measurable amount of heat (on the order of 35 J/mol) (17-19) establishes hexagonal ice as the equilibrium structure above 170 K. Below 170 K no phase transformation has been observed, allowing for the poss...

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Section: Resultssupporting

confidence: 55%

Formation of hexagonal and cubic ice during low-temperature growth

Thürmer

Nie

2013

Proc. Natl. Acad. Sci. U.S.A.

109

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“…Nie et al's recent examination of water on Pt(111) 13 has provided a new way to think about wetting layer structures. Their STM data showed that the first water layer on Pt(111) has two levels, and that its periodicity reflects an ordered arrangement of patches of low-lying water molecules.…”

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confidence: 99%

“…A natural way to add them without breaking bonds is to incorporate them in boundaries between clusters of differently rotated hexagons. 13 Replacing four water molecules arranged in a "Y" by a hexagon converts a flat, hexagonally-coordinated mesh of H 2 O into a two-level mesh, with hexagons of flat-lying H 2 O connected by 5-and 7-fold rings of molecules, to chains of dangling-H molecules in hexagons misoriented azimuthally by 30…”

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confidence: 99%

Adsorbed water-molecule hexagons with unexpected rotations in islands on Ru(0001) and Pd(111)

et al. 2012

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“…Due to the relative strength and particular directionality of interactions between water molecules, which are delicately balanced against molecule-surface interactions, the structures of water monolayers on various surfaces exhibit surprising diversity. This has been recently demonstrated in scanning tunnelling microscopy (STM) studies [5][6][7][8] , which allow direct visualization of hydrogen bonding networks. The most detailed insight into water adsorption has been achieved for single-crystal metal surfaces, where the structure of water layers is determined mainly by the dimensions of the surface unit cell and the strength of metal-oxygen bonding 6 .…”

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confidence: 99%

Water clustering on nanostructured iron oxide films

et al. 2014

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The adhesion of water to solid surfaces is characterized by the tendency to balance competing molecule-molecule and molecule-surface interactions. Hydroxyl groups form strong hydrogen bonds to water molecules and are known to substantially influence the wetting behaviour of oxide surfaces, but it is not well-understood how these hydroxyl groups and their distribution on a surface affect the molecular-scale structure at the interface. Here we report a study of water clustering on a moiré-structured iron oxide thin film with a controlled density of hydroxyl groups. While large amorphous monolayer islands form on the bare film, the hydroxylated iron oxide film acts as a hydrophilic nanotemplate, causing the formation of a regular array of ice-like hexameric nanoclusters. The formation of this ordered phase is localized at the nanometre scale; with increasing water coverage, ordered and amorphous water are found to coexist at adjacent hydroxylated and hydroxyl-free domains of the moiré structure.

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Pentagons and Heptagons in the First Water Layer on Pt(111)

Cited by 229 publications

References 21 publications

Formation of hexagonal and cubic ice during low-temperature growth

Formation of hexagonal and cubic ice during low-temperature growth

Adsorbed water-molecule hexagons with unexpected rotations in islands on Ru(0001) and Pd(111)

Water clustering on nanostructured iron oxide films

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