Experimental and theoretical bond critical point properties for model electron density distributions for earth materials |
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| Authors: | G V Gibbs D F Cox K M Rosso A Kirfel T Lippmann P Blaha K Schwarz |
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| Institution: | (1) Departments of Geosciences, Materials Science and Engineering and Mathematics, Virginia Tech, Blacksburg, VA 24061, USA;(2) Department of Chemical Engineering, Virginia Tech, Blacksburg, VA 24061, USA;(3) W.R. Wiley Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, P.O. Box 999, KB-96, Richland, WA 99352, USA;(4) Mineralogisch-Petrologisches Institut, Universität Bonn, Poppelsdorfer Schloss, 53115 Bonn, Germany;(5) GKSS, Max-Planck-Strasse, 21502 Geesthacht, Germany;(6) Institut für Materialchemie, Technische Universität Wien, Getreidemarkt 9/156-TC, 1060 Wien, Austria |
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| Abstract: | Generalized X-ray scattering factor model experimental electron density distributions and bond critical point, bcp, properties generated in recent studies for the earth materials stishovite, forsterite, fayalite and cuprite with high energy single crystal synchrotron X-ray diffraction data and those generated with high resolution diffraction data for coesite and senarmonite were found to be adequate and in relatively good agreement, ~5% on average, with those calculated with quantum chemical methods with relatively robust basis sets. High resolution low energy single crystal diffraction data, recorded for the molecular sieve AlPO4-15, were also found to yield model electron density distribution values at the bcp points for the AlO and PO bonded interactions that are in relatively good to moderately good agreement with the theoretical values, but the Laplacian values of the distribution at the points for the two bonded interactions were found to be in relatively poor agreement. In several cases, experimental bcp properties, generated with conventional low energy X-ray diffraction data for several rock forming minerals, were found overall to be in poorer agreement with the theoretical properties. The overall agreement between theoretical bcp properties generated with computational quantum methods and experimental properties generated with synchrotron high energy radiation not only provides a basis for using computational strategies for studying and modeling structures and their electron density distributions, but it also provides a basis for improving our understanding of the crystal chemistry and bonded interactions for earth materials. Theoretical bond critical point properties generated with computational quantum methods are believed to rival the accuracy of those determined experimentally. As such the calculations provide a powerful and efficient method for evaluating electron density distributions and the bonded interactions for a wide range of earth materials.Dedicated to Professor Robert F. Stewart of Carnegie Mellon University on his retirement for his brilliant and original work modeling electron density distributions. |
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| Keywords: | Synchrotron diffraction data Silica polymorphs Forsterite AlPO4-15 Fibrous zeolites Cuprite Danburite Bromellite Senarmonite |
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