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New short-range order data are presented for equilibrium and undercooled liquids of Ti and Ni. These were obtained from in situ synchrotron x-ray diffraction measurements of electrostatically levitated droplets. While the short-range order of liquid Ni is icosahedral, consistent with Frank's hypothesis, significantly distorted icosahedral order is observed in liquid Ti. This is the first experimental observation of distorted icosahedral short-range order in any liquid, although this has been predicted by theoretical studies on atomic clusters.  相似文献   
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Nuclear quantum effects in finite temperature simulations of molecular clusters are determined by taking advantage of a recently developed method based on the Feynman Path Integral. The structural and thermodynamic properties, including the nuclear quantum effects are determined for three Stockmayer clusters. The ionic system contain a lithium ion solvated by six strong dipoles and 12 weaker ones. The presence of the ion in the mixed Stockmayer cluster drastically enhances the fluxional nature of the less polar components which occupy the second solvation layer, whereas the neutral counterpart has the effect of reducing it. The nuclear quantum effects are significant at room temperature and above for the solvated ionic system. These are attributable to two factors: (a) the lightness of the lithium ion and (b) the stiffness of the ion-dipole interactions. At 300 K, the difference between the fully converged quantum and the classical heat capacities is about 1.3 KB for the ionic cluster. This difference is about 10 SDs obtained from 95% confidence estimates of the statistical fluctuations. Cubic convergence is confirmed for temperatures as low as 50 K by regression analysis. The nuclear quantum effects do not change the peak melting temperature of the cluster.  相似文献   
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To explain the unusual stability of undercooled liquids against crystallization, Frank hypothesized that the local structures of undercooled liquids contain a significant degree of icosahedral short-range order, which is incompatible with long-range periodicity. We present here the first direct experimental demonstration of Frank's complete hypothesis, showing a correlation between the nucleation barrier and a growing icosahedral short-range order with decreasing temperature in a Ti39.5Zr39.5Ni21 liquid. A new experimental facility, BESL (Beamline Electrostatic Levitation), was developed to enable the synchrotron x-ray structural studies on deeply undercooled, reactive liquids.  相似文献   
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