软质多孔晶体第一性原理NPT分子动力学的挑战：MIL-53（Ga）的研究
Challenges in first-principles NPT molecular dynamics of soft porous crystals: A case study on MIL-53(Ga)
摘要：
软多孔晶体对具有灵活尺寸和形状的模拟单元的分子动力学模拟提出挑战（即，在《不扩散条约》总体框架内），因为它们的框架对微小的外部刺激非常敏感。因此，所有的相互作用必须非常精确地描述，以获得正确的平衡结构。在这里，我们报告的纳米多孔金属有机框架MIL-53（Ga），它经历了一个大幅度的转变之间的窄和大孔相时，温度的变化的方法研究。由于这个系统还没有被调查的密度泛函理论（DFT）为基础的NPT模拟到目前为止，我们仔细检查的收敛应力张量的计算参数。此外，我们证明了色散相互作用的重要性，并测试两种不同的方式将它们纳入DFT框架。因此，我们提出了两个计算方案，准确地描述了窄和大孔相的材料，分别。这些方案可以用于未来的工作中的微妙的相互作用之间的吸附在纳米孔和结构的主体材料的灵活性。
英文摘要：
Soft porous crystals present a challenge to molecular dynamics simulations with flexible size and shape of the simulation cell (i.e., in the NPT ensemble), since their framework responds very sensitively to small external stimuli. Hence, all interactions have to be described very accurately in order to obtain correct equilibrium structures. Here, we report a methodological study on the nanoporous metal-organic framework MIL-53(Ga), which undergoes a large-amplitude transition between a narrow- and a large-pore phase upon a change in temperature. Since this system has not been investigated by density functional theory (DFT)-based NPT simulations so far, we carefully check the convergence of the stress tensor with respect to computational parameters. Furthermore, we demonstrate the importance of dispersion interactions and test two different ways of incorporating them into the DFT framework. As a result, we propose two computational schemes which describe accurately the narrow- and the large-pore phase of the material, respectively. These schemes can be used in future work on the delicate interplay between adsorption in the nanopores and structural flexibility of the host material.
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