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Using variational Monte Carlo and a simple explicitly correlated wave function we have computed the Born-Oppenheimer energy of the H2 ground state (X 1Sigmag+) at 24 internuclear distances. We have also calculated the diagonal correction to the Born-Oppenheimer approximation and the lowest-order relativistic corrections at each distance using variational Monte Carlo techniques. The nonadiabatic values are evaluated from numerical derivatives of the wave function with respect to the nuclear coordinates. With this potential energy surface we have computed several of the lowest vibrational-rotational energies for this system. Our results are in good agreement with the best values found in the literature. 相似文献
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Dupont-Gillain CC Jacquemart I Rouxhet PG 《Colloids and surfaces. B, Biointerfaces》2005,43(3-4):179-186
In the last years, adsorbed collagen was shown to form layers with a supramolecular organization depending on the substrate surface properties and on the preparation procedure. If the concentration of collagen and the duration of adsorption are sufficient, fibrillar collagen structures are formed, corresponding to assemblies of a few molecules. This occurs more readily on hydrophobic compared to hydrophilic surfaces. This study aims at understanding the origin of such fibrillar structures and in particular at determining whether they result from the deposition of fibrils formed in solution or from the building of assemblies at the interface. Therefore, type I collagen solutions with an increasing degree of aggregation were prepared, using the “neutral-start” approach, by ageing pH 5.8 solutions at 37 °C for 15 min, 2 or 7 days. The obtained solutions were used to investigate the influence of collagen aggregation in solution on the supramolecular organization of adsorbed collagen layers, which was characterized by X-ray photoelectron spectroscopy and atomic force microscopy. Polystyrene and plasma-oxidized polystyrene were chosen as substrates for the adsorption. The size and the density of collagen fibrils at the interface decreased upon increasing the degree of aggregation of collagen in solution. This is explained by a competitive adsorption process between monomers and aggregates of the solution, turning at the advantage of the monomers. More aggregated solutions, which are thus depleted in free monomers, behave like less concentrated solutions, i.e. lead to a lower adsorbed amount and less fibril formation at the interface. This study shows that the supramolecular fibrils observed in adsorbed collagen layers, especially on hydrophobic substrates, are not formed in the solution, prior to adsorption, but are built at the interface, through the assembly of free segments of adsorbed molecules. 相似文献
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Abstract Organic-inorganic composites (OICs) were prepared via the in-situ polymerization of an organically (phenyl) substituted trialkoxysilane, phenyltriethoxysilane (PhTEOS), in the presence of poly(vinyl acetate) (PVAc). The mechanical reinforcement above T g previously observed in OICs of unfunctionalized organic polymers such as PVAc with acid catalyzed in-situ polymerized tetraalkoxysilane was not observed when the tetraalkoxysilane was replaced with PhTEOS. Although both systems are optically transparent and both exhibit a high degree of hydrogen bonding between the carbonyl of PVAc and the residual hydroxyls of the silicate, the polymerization of the alkoxide is different. The tetra-functional alkoxide polymerizes to form a load-supporting silicate network, leading to a high plateau in the tensile modulus above T g, whereas the trifunctional alkoxide reacts to form primarily low molecular weight oligomers. These increase the T g of the PVAc but do not provide mechanical reinforcement. 相似文献
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Thomas Courant Valrie Gaëlle Roullin Cyril Cadiou Maït Callewaert Marie Christine Andry Christophe Portefaix Christine Hoeffel Marie Christine deGoltstein Marc Port Sophie Laurent Luce Vander Elst Robert Muller Michaël Molinari Franoise Chuburu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2012,124(36):9253-9256