Journal of Molecular Modeling ( IF 2.1 ) Pub Date : 2023-11-21 , DOI: 10.1007/s00894-023-05781-4 Surajit Guin 1 , Sasthi Charan Halder 1 , Sourav Ranjan Ghosh 1, 2 , Atish Dipankar Jana 1, 3
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Context
Dynamic metal nanoclusters have become a hot area of research in the field of nanoscience and nanotechnology due to their potential applications in micro devices. One such dynamic cluster is a quasi-planar ground state (GS) Al13+ cluster which exhibits an electric field driven up and down flipping motion of the flexible tail which oscillates with respect to the mean plane. A Car-Parrinello molecular dynamics (CPMD) simulation has been carried out to understand the nature of dynamics of the cluster. CPMD simulation study reveals that the flexible tail region of the Al13+ isomeric system (two ground states M1, M2 and a transition state TS connecting them) can be engaged in a systematic up down flipping motion by the application of a transverse electric field. A saw tooth electric field of amplitude 5.19 V/nm is sufficient to induce the up-and-down flipping oscillation of the cluster, which has an average oscillation frequency of around 20 THz. AIM, NICS and AdNDP analyses also have been carried out to understand the fluxional nature of the cluster from the electronic structural perspective. Electronic structural analysis of selected optimized intermediate states in the presence of transverse electric field has also been analyzed to correlate the electronic structure with the dynamic nature of the cluster.
Methods
Single-point energies of all intermediate states between two minima of Al13+ clusters connected through a transition state cluster. Optimized geometries of Al13+ clusters in the presence of electric field of different strengths have been carried out by using the Gaussian 03 package. 6–311 + G(d) basis set and B3LYP hybrid density functional have been utilized for these studies. To establish the flipping motion, Car-Parrinello molecular dynamics (CPMD) has been performed using the cp.x module of the Quantum ESPRESSO 6.3.0 program package using the Perdew-Burke-Ernzerhof (PBE) functional, plane-wave basis set and ultrasoft pseudopotentials. ORTEP-3 and POV ray-3.7 software packages have been used for visualization and graphics generation. Atoms in molecule (AIM), Adaptive Natural Density Partitioning (AdNDP) analysis have been carried out using Multiwfn 3.7 program package.
中文翻译：
电场驱动Al13+团簇系统柔性尾部的上下运动——纳米级鳍状肢
语境
动态金属纳米团簇因其在微型器件中的潜在应用而成为纳米科学和纳米技术领域的研究热点。一种这样的动态团簇是准平面基态（GS）Al 13 +团簇，其表现出电场驱动柔性尾部的上下翻转运动，该柔性尾部相对于平均平面振荡。为了了解团簇动力学的本质，我们进行了 Car-Parrinello 分子动力学 (CPMD) 模拟。 CPMD模拟研究表明，Al 13 +异构系统的柔性尾区（两个基态M1、M2和连接它们的过渡态TS）可以通过施加横向电场进行系统的上下翻转运动。振幅为5.19 V/nm的锯齿状电场足以引起团簇的上下翻转振荡，其平均振荡频率约为20 THz。还进行了 AIM、NICS 和 AdNDP 分析，以从电子结构的角度了解团簇的流动性质。还对存在横向电场的情况下选定的优化中间态的电子结构进行了分析，以将电子结构与团簇的动态性质相关联。
方法
通过过渡态簇连接的 Al 13 +簇的两个最小值之间的所有中间态的单点能量。使用Gaussian 03 软件包对不同强度电场下Al 13 +团簇的几何形状进行了优化。 6–311 + G(d) 基组和 B3LYP 混合密度泛函已用于这些研究。为了建立翻转运动，使用 Quantum ESPRESSO 6.3.0 程序包的 cp.x 模块使用 Perdew-Burke-Ernzerhof (PBE) 函数、平面波基组和超软赝势。 ORTEP-3 和 POV ray-3.7 软件包已用于可视化和图形生成。使用 Multiwfn 3.7 程序包进行分子中原子 (AIM)、自适应自然密度分区 (AdNDP) 分析。
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