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 229                 <prim:type>article</prim:type>
 230                 <prim:title>Glassy nature of water in an ultraconfining disordered material: the case of calcium-silicate-hydrate</prim:title>
 231                 <prim:creator>Youssef, Mostafa ; Pellenq, Roland J-M ; Yildiz, Bilge</prim:creator>
 232                 <prim:ispartof>Journal of the American Chemical Society, Mar, 2011, Vol.133(8), p.2499-510</prim:ispartof>
 233                 <prim:identifier><![CDATA[<b>E-ISSN:</b> 1520-5126 ; <b>ISSN:</b> 0002-7863 ; <b>PMID:</b> 21294516]]></prim:identifier>
 234                 <prim:subject>Calcium -- chemistry; Silicates -- chemistry; Water -- chemistry</prim:subject>
 235                 <prim:description>We present the structural and dynamic nature of water ultraconfined in the quasi-two-dimensional nanopores of the highly disordered calcium-silicate-hydrate (C-S-H), the major binding phase in cement. Our approach is based on classical molecular simulations. We demonstrate that the C-S-H nanopore space is hydrophilic, particularly because of the nonbridging oxygen atoms on the disordered silicate chains which serve as hydrogen-bond acceptor sites, directionally orienting the hydrogen atoms of the interfacial water molecules toward the calcium-silicate layers. The water in this interlayer space adopts a unique multirange structure: a distorted tetrahedral coordination at short range up to 2.7 Å, a disordered structure similar to that of dense fluids and supercooled phases at intermediate range up to 4.2 Å, and persisting spatial correlations through dipole-dipole interactions up to 10 Å. A three-stage dynamics governs the mean square displacement (MSD) of water molecules, with a clear cage stage characteristic of the dynamics in supercooled liquids and glasses, consistent with its intermediate-range structure identified here. At the intermediate time scales corresponding to the β-relaxation of glassy materials, coincident with the cage stage in MSD, the non-Gaussian parameter indicates a significant heterogeneity in the translational dynamics. This dynamic heterogeneity is induced primarily because of the heterogeneity in the distribution of hydrogen bond strengths. The strongly attractive interactions of water molecules with the calcium silicate walls serve to constrain their motion. Our findings have important implications on describing the cohesion and mechanical behavior of cement from its setting to its aging.</prim:description>
 236                 <prim:language>eng</prim:language>
 237                 <prim:source>MEDLINE (NLM)</prim:source>
 238                 <prim:lds50>peer_reviewed</prim:lds50>
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 242                 <prim:openurl>$$Topenurl_article</prim:openurl>
 243                 <prim:backlink>$$Uhttp://pubmed.gov/21294516$$DView this record at the National Library of Medicine site.</prim:backlink>
 244                 <prim:openurlfulltext>$$Topenurlfull_article</prim:openurlfulltext>
 245                 <prim:addlink>$$Uhttp://primo-central-3.saas.exlibrisgroup.com:1701/primo_library/libweb/aboutMedline.html$$DView the National Library of Medicine Copyright Statement</prim:addlink>
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 248                 <prim:creatorcontrib>Youssef, Mostafa</prim:creatorcontrib>
 249                 <prim:creatorcontrib>Pellenq, Roland J-M</prim:creatorcontrib>
 250                 <prim:creatorcontrib>Yildiz, Bilge</prim:creatorcontrib>
 251                 <prim:title>Glassy nature of water in an ultraconfining disordered material: the case of calcium-silicate-hydrate.</prim:title>
 252                 <prim:description>We present the structural and dynamic nature of water ultraconfined in the quasi-two-dimensional nanopores of the highly disordered calcium-silicate-hydrate (C-S-H), the major binding phase in cement. Our approach is based on classical molecular simulations. We demonstrate that the C-S-H nanopore space is hydrophilic, particularly because of the nonbridging oxygen atoms on the disordered silicate chains which serve as hydrogen-bond acceptor sites, directionally orienting the hydrogen atoms of the interfacial water molecules toward the calcium-silicate layers. The water in this interlayer space adopts a unique multirange structure: a distorted tetrahedral coordination at short range up to 2.7 Å, a disordered structure similar to that of dense fluids and supercooled phases at intermediate range up to 4.2 Å, and persisting spatial correlations through dipole-dipole interactions up to 10 Å. A three-stage dynamics governs the mean square displacement (MSD) of water molecules, with a clear cage stage characteristic of the dynamics in supercooled liquids and glasses, consistent with its intermediate-range structure identified here. At the intermediate time scales corresponding to the β-relaxation of glassy materials, coincident with the cage stage in MSD, the non-Gaussian parameter indicates a significant heterogeneity in the translational dynamics. This dynamic heterogeneity is induced primarily because of the heterogeneity in the distribution of hydrogen bond strengths. The strongly attractive interactions of water molecules with the calcium silicate walls serve to constrain their motion. Our findings have important implications on describing the cohesion and mechanical behavior of cement from its setting to its aging.</prim:description>
 253                 <prim:subject>Calcium -- chemistry</prim:subject>
 254                 <prim:subject>Silicates -- chemistry</prim:subject>
 255                 <prim:subject>Water -- chemistry</prim:subject>
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 276                 <prim:creationdate>2011</prim:creationdate>
 277                 <prim:author>Youssef, Mostafa ; Pellenq, Roland J-M ; Yildiz, Bilge</prim:author>
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 282                 <prim:topic>Calcium -- chemistry</prim:topic>
 283                 <prim:topic>Silicates -- chemistry</prim:topic>
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 343                 <prim:abstract>We present the structural and dynamic nature of water ultraconfined in the quasi-two-dimensional nanopores of the highly disordered calcium-silicate-hydrate (C-S-H), the major binding phase in cement. Our approach is based on classical molecular simulations. We demonstrate that the C-S-H nanopore space is hydrophilic, particularly because of the nonbridging oxygen atoms on the disordered silicate chains which serve as hydrogen-bond acceptor sites, directionally orienting the hydrogen atoms of the interfacial water molecules toward the calcium-silicate layers. The water in this interlayer space adopts a unique multirange structure: a distorted tetrahedral coordination at short range up to 2.7 Å, a disordered structure similar to that of dense fluids and supercooled phases at intermediate range up to 4.2 Å, and persisting spatial correlations through dipole-dipole interactions up to 10 Å. A three-stage dynamics governs the mean square displacement (MSD) of water molecules, with a clear cage stage characteristic of the dynamics in supercooled liquids and glasses, consistent with its intermediate-range structure identified here. At the intermediate time scales corresponding to the β-relaxation of glassy materials, coincident with the cage stage in MSD, the non-Gaussian parameter indicates a significant heterogeneity in the translational dynamics. This dynamic heterogeneity is induced primarily because of the heterogeneity in the distribution of hydrogen bond strengths. The strongly attractive interactions of water molecules with the calcium silicate walls serve to constrain their motion. Our findings have important implications on describing the cohesion and mechanical behavior of cement from its setting to its aging.</prim:abstract>
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 546                 <description>X-ray absorption spectroscopy and x-ray Raman scattering were used to probe the molecular arrangement in the first coordination shell of liquid water. The local structure is characterized by comparison with bulk and surface of ordinary hexagonal ice Ih and with calculated spectra. Most molecules in liquid water are in two hydrogen-bonded configurations with one strong donor and one strong acceptor hydrogen bond in contrast to the four hydrogen-bonded tetrahedral structure in ice. Upon heating from 25 degrees C to 90 degrees C, 5 to 10% of the molecules change from tetrahedral environments to two hydrogen-bonded configurations. Our findings are consistent with neutron and x-ray diffraction data, and combining the results sets a strong limit for possible local structure distributions in liquid water. Serious discrepancies with structures based on current molecular dynamics simulations are observed.</description>
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 620                 <abstract>X-ray absorption spectroscopy and x-ray Raman scattering were used to probe the molecular arrangement in the first coordination shell of liquid water. The local structure is characterized by comparison with bulk and surface of ordinary hexagonal ice Ih and with calculated spectra. Most molecules in liquid water are in two hydrogen-bonded configurations with one strong donor and one strong acceptor hydrogen bond in contrast to the four hydrogen-bonded tetrahedral structure in ice. Upon heating from 25 degrees C to 90 degrees C, 5 to 10% of the molecules change from tetrahedral environments to two hydrogen-bonded configurations. Our findings are consistent with neutron and x-ray diffraction data, and combining the results sets a strong limit for possible local structure distributions in liquid water. Serious discrepancies with structures based on current molecular dynamics simulations are observed.</abstract>
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