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首页> 外文期刊>The journal of physical chemistry, B. Condensed matter, materials, surfaces, interfaces & biophysical >Melting in Large Sodium Clusters: An Orbital-Free Molecular Dynamics Study
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Melting in Large Sodium Clusters: An Orbital-Free Molecular Dynamics Study

机译:大型钠团簇中的熔融:无轨道分子动力学研究

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摘要

The melting-like transition in sodium clusters NaN, with N = 55, 92, and 142, is studied by using constant-energy molecular dynamics simulations. An orbital-free version of the Car-Parrinello technique is used that scales linearlywith system size, allowing for investigations of the thermal behavior of large clusters.The ground-state isomer of Na_(142) (an incomplete three-shell icosahedron) melts in two steps: the first (at approx 240K) is characterized by the high mobility of atoms located on the cluster surface, and the second,melting (at approx 270 K) involves diffusive motion of all of the atoms across the cluster. For the case of Na_(92), the icosahedral structure has a larger number of surface vacancies and melts in two well-separated steps, wil surface melting at approx 130 K and homogeneous melting at approx 240 K. Na55, a complete two-shell icosahedra. melts in a single stage at approx 190 K. Our results on homogeneous melting for Na1.and Na_(92) are in excell~ agreement with recent experimental determinations of melting temperatures and latent heats. However, tlu experimentally observed enhancement of the melting temperature around N_(55) is not reproduced by tiu calculations.
机译:通过使用恒定能量分子动力学模拟研究了N = 55、92和142的钠簇NaN中的熔融样转变。使用Car-Parrinello技术的无轨道版本,该轨道随系统大小线性缩放,从而可以研究大型团簇的热行为.Na_(142)(不完整的三壳二十面体)的基态异构体在分两个步骤:第一个步骤(约240K)的特征是位于团簇表面的原子具有很高的迁移率,第二个步骤是熔化(约270K)涉及所有原子在整个团簇中的扩散运动。对于Na_(92)而言,二十面体结构具有较大的表面空位,并且在两个完全分开的步骤中熔化,即约130 K的表面熔融和约240 K的均匀熔融。Na55,完整的两层壳二十面体。在大约190 K的温度下单步熔化。我们对Na1和Na_(92)进行均匀熔化的结果与最近对熔化温度和潜热的实验测定结果非常一致。然而,通过实验观察到的,在t_(55)附近的熔化温度的提高并未通过tiu计算得到再现。

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