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Structures of quartz (100)- and (101)-water interfaces determined by x-ray reflectivity and atomic force microscopy of natural growth surfaces |
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| Authors: | Michel L Schlegel Kathryn L Nagy Paul FenterNeil C Sturchio |
| Institution: | 1 Department of Geological Sciences, University of Colorado, 399 UCB, Boulder, CO 80309, USA 2 Environmental Research Division, Argonne National Laboratory, Argonne, IL 60439, USA 3 Department of Earth and Environmental Sciences, University of Illinois at Chicago, Chicago, IL 60607, USA |
| Abstract: | The structures of prismatic (100) and pyramidal (101) growth faces of natural quartz crystals, and their modification upon annealing at T ≤ 400°C were investigated ex situ by atomic force microscopy (AFM) and in water by high-resolution X-ray reflectivity. AFM images revealed the presence of ∼ 0.1 to 1 μm-wide flat terraces delimited by steps of one to several unit cells in height. These steps follow approximately directions given by the intersection of growth faces. Modeling of X-ray reflectivity data indicates that surface silica groups on flat terraces have only one free Si-O bond each (presumably hydroxylated), except for some having two free Si-O bonds observed on a single (100) surface. Vertical relaxation of atomic positions (< 0.4 Å for terminal oxygens and < 0.2 Å for silicon and oxygen atoms fully coordinated to structural tetrahedra) is limited to a depth of 14 Å. Electron density profiles for all measured interfaces are consistent with a single layer of adsorbed water, with no evidence for additional organization of water molecules into distinct layers extending into the bulk solution. Similar interfacial structures were observed for natural and annealed surfaces of identical crystallographic orientation, indicating that extensive reconstruction of the silica network at the quartz surface did not occur under the annealing conditions. |
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