论文标题

Cu $ _ {38} $群集在有限温度下的结构和稳定性

Structures and stability of the Cu$_{38}$ cluster at finite temperature

论文作者

Castillo-Quevedo, César, Paredes-Sotelo, Edgar, Buelna-García, Carlos Emiliano, Hoil-Canul, Edwin Rene, Mis-May, Jhonny Robert, Barrios-Díaz, Jarbin, Martin-del-Campo-Solis, Martha Fabiola, Zamora-Gonzalez, Edgar, López-Sánchez, Adolfo, Cob-Cantu, Jesús Ramón, Briceño-Mena, Jorge, Agustín-Argüello, Freddy Francisco, López-Luke, Tzarara, Martínez-Guajardo, Gerardo, Cabellos, José Luis

论文摘要

Cu $ _ {38} $ nanocluster的UV可见和IR属性在很大程度上取决于温度。密度功能理论和纳米热动力学可以组合以近似方式计算异构体及其光谱特性的几何优化。在本文中,我们研究了Cu $ _ {38} $簇的熵驱动的异构体分布以及温度对其UV可见和IR光谱的影响。使用两阶段策略来识别最低能量结构及其低能邻居,对CU38的潜在和自由能表面进行了广泛的全球搜索。温度对紫外线和红外光谱的影响是通过玻尔兹曼概率来考虑的。在有限温度下,每个异构体的计算出的紫外可见度和红外光谱乘以其相应的玻尔兹曼重量。然后,将它们求和在一起,以产生最终的温度依赖性,玻尔兹曼加权紫外线和红外光谱。此外,还执行了Cu $ _ {38} $纳米升级的分子动力学模拟,以洞悉系统动力学,并通过原子分辨率制作系统的三维电影。我们的结果表明,在CU38簇的绝对温度下的热种群以及在高温下主导的无序结构。

The UV-visible and IR properties of the Cu$_{38}$ nanocluster depend to a great extent on the temperature. Density functional theory and nanothermodynamics can be combined to compute the geometrical optimization of isomers and their spectroscopic properties in an approximate manner. In this article, we investigate entropy-driven isomer distributions of Cu$_{38}$ clusters and the effect of temperature on their UV-visible and IR spectra. An extensive, systematic global search is performed on the potential and free energy surfaces of Cu38 using a two-stage strategy to identify the lowest-energy structure and its low-energy neighbors. The effects of temperature on the UV and IR spectra are considered via Boltzmann probability. The computed UV-visible and IR spectrum of each isomer is multiplied by its corresponding Boltzmann weight at finite temperature. Then, they are summed together to produce a final temperature-dependent, Boltzmann-weighted UV-visible and IR spectrum. Additionally, Molecular Dynamics simulation of the Cu$_{38}$ nanocluster was performed to gain insight into the system dynamics and make a three-dimensional movie of the system with atomistic resolution. Our results show the thermal populations at the absolute temperature of Cu38 cluster, and the disordered structure that dominates at high temperatures.

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