Solid water clusters in the size range of tens–thousands of H<sub>2</sub>O: a combined computational/spectroscopic outlook

Buch, V.; Bauerecker, S.; Devlin, J. Paul; Buck, U.; Kazimirski, J. K.

doi:10.1080/01442350412331316124

Cited by 224 publications

(343 citation statements)

References 189 publications

(305 reference statements)

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“…It is wellknown that hydrogen-bonded νOH exhibits higher band intensity than non-hydrogen-bonded νOH. 20 Hence, the experimentally observed νOH band intensity increase can only be interpreted as arising from an increase in the degree of hydrogen bonding in the deposited H 2 O film.…”

Section: Resultsmentioning

confidence: 99%

Peeling the astronomical onion

Rosu-Finsen

Marchione

Salter

et al. 2016

Phys. Chem. Chem. Phys.

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Journal Name ARTICLEThis journal is © The Royal Society of Chemistry 20xxJ. Name., 2013, 00, 1-3 | 1 Water ice is the most abundant solid in the Universe. Understanding the formation, structure and multiplicity of physicochemical roles for water ice in the cold, dense interstellar environments in which it is predominantly observed is a crucial quest for astrochemistry as these are regions active in star and planet formation. Intuitively, we would expect the mobility of water molecules deposited or synthesised on dust grain surfaces at temperatures below 50 K to be very limited. This work delves into the thermally-activated mobility of H2O molecules on model interstellar grain surfaces. The energy required to initiate this process is studied by reflection-absorption infrared spectroscopy of small quantities of water on amorphous silica and highly oriented pyrolytic graphite surfaces as the surface is annealed. Strongly nonArrhenius behaviour is observed with an activation energy of 2 kJ mol -1 on the silica surface below 25 K and 0 kJ mol -1 on both surfaces between 25 and 100 K. The astrophysical implication of these results is that on timescales shorter than that estimated for the formation of a complete monolayer of water ice on a grain, aggregation of water ice will result in a nonuniform coating of water, hence leaving bare grain surface exposed. Other molecules can thus be formed or adsorbed on this bare surface.

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Section: Resultsmentioning

confidence: 99%

Peeling the astronomical onion

Rosu-Finsen

Marchione

Salter

et al. 2016

Phys. Chem. Chem. Phys.

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“…In neutral water clusters, the onset of crystallinity occurs somewhere in the size range from 200 to 1000 water molecules 29 , i.e., at much larger cluster sizes than probed here. Smaller water clusters correspond to quasi spherical nanoparticles with a crystal interior and a disordered "reconstructed" surface 30 , while even smaller clusters contain only "surface" water molecules. The reconstruction of the cluster surface may lead to a weakening of the hydrogen bonding network and thus a red shift of the librational band in the present IRMPD spectra compared to the IR spectrum of bulk ice.…”

Section: Manuscriptmentioning

confidence: 99%

Vibrational spectroscopy of hydrated electron clusters(H2O)15–50− via infrared multiple photon dissociation

Asmis

Santambrogio

Zhou³

et al. 2007

The Journal of Chemical Physics

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Infrared multiple photon dissociation spectra for size-selected water cluster anions (H2O)n−, n=15–50, are presented covering the frequency range of 560–1820cm−1. The cluster ions are trapped and cooled by collisions with ambient He gas at 20K, with the goal of defining the cluster temperature better than in previous investigations of these species. Signal is seen in two frequency regions centered around 700 and 1500–1650cm−1, corresponding to water librational and bending motions, respectively. The bending feature associated with a double-acceptor water molecule binding to the excess electron is clearly seen up to n=35, but above n=25; this feature begins to blueshift and broadens, suggesting a more delocalized electron binding motif for the larger clusters in which the excess electron interacts with multiple water molecules.

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“…It has long been recognized that the adsorption properties depend on the structure of the ice surface (6)(7)(8)(9). However, it is still striking to see that many properties of ice surfaces vary greatly even on a prefect ice surface where the oxygen atoms are ordered in a hexagonal lattice (10)(11)(12)(13)). Yet, due to the complexity of the surface structure at the atomic level, our understandings of the activity and adsorption property on the ice surface are still far from consistent and complete.…”

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confidence: 99%

Role of proton ordering in adsorption preference of polar molecule on ice surface

Sun

Pan

et al. 2012

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

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Adsorption of polar monomers on ice surface, relevant to the physical/chemical reaction in ice clouds as well as growth of ice, remains an open issue partially due to the unusual surface characteristics with protons at the top layer of ice. Using first-principle calculations, we explore the adsorption properties of ice surface in terms of a surface proton order parameter, which characterizes the inhomogeneity of the dangling atoms on ice surface. We show that, due to an effective electric field created by dangling OH bonds and lone pairs of water molecules not only directly neighboring but also further away from the adsorbed polar molecule on the ice surface, the adsorption energy of polar monomer on ice surface exhibits large variance and a strong correlation with the proton order parameter of ice surface. Our results about the positive correlation between the inhomogeneity of ice surface and adsorption energies suggest that the physical/chemical reactions as well as the growth of ice may prefer to occur firstly on surfaces with larger proton order parameter.surface science | ice basal surface | ice growth | ice basal plane I ce, one of the most abundant materials on earth, plays an important role in interstellar phenomena, life in the cryosphere and global climate (1-3). Adsorption on ice surface, especially hexagonal ice, is related to the fundamental question of how ice particles grow into hexagonal ice crystal or snow flakes, and what kind of roles it plays for the reactive and catalytic properties of atmospheric ice associated with environment-related issues (1-4). For instance, the ice surface acts as a catalyst in heterogeneous physical/chemical reactions leading to the destruction of ozone (5). It has long been recognized that the adsorption properties depend on the structure of the ice surface (6-9). However, it is still striking to see that many properties of ice surfaces vary greatly even on a prefect ice surface where the oxygen atoms are ordered in a hexagonal lattice (10-13). Yet, due to the complexity of the surface structure at the atomic level, our understandings of the activity and adsorption property on the ice surface are still far from consistent and complete.At interfaces, the Bernal-Fowler-Pauling ice rule (14, 15) cannot be obeyed; that is, nearest neighboring water molecules cannot satisfy all hydrogen bonds, thus forming dangling protons and lone pairs. Recent works (16-18) have shown that the inhomogeneity of dangling atoms, which can be characterized by a proton order parameter (17), is important for the energies of water ice surfaces (17,18). This order parameter, C OH , characterizing the arrangement of dangling OH bonds on the ice surface (17), is defined aswhere N OH is the total number of dangling OH bonds on the surface and c i is the number of the nearest neighboring dangling OH bonds around the ith OH bond. For the ice slab without dipole moment perpendicular to the surface, the order parameter ranges from 2 to 6 (17). We note that the most ordered dangling OH distribution on...

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Solid water clusters in the size range of tens–thousands of H₂O: a combined computational/spectroscopic outlook

Cited by 224 publications

References 189 publications

Peeling the astronomical onion

Peeling the astronomical onion

Vibrational spectroscopy of hydrated electron clusters(H2O)15–50− via infrared multiple photon dissociation

Role of proton ordering in adsorption preference of polar molecule on ice surface

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Solid water clusters in the size range of tens–thousands of H2O: a combined computational/spectroscopic outlook

Cited by 224 publications

References 189 publications

Peeling the astronomical onion

Peeling the astronomical onion

Vibrational spectroscopy of hydrated electron clusters(H2O)15–50− via infrared multiple photon dissociation

Role of proton ordering in adsorption preference of polar molecule on ice surface

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Solid water clusters in the size range of tens–thousands of H₂O: a combined computational/spectroscopic outlook