神经网络势预测C60分子晶体的结构演化,Advanced Functional Materials

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神经网络势预测C60分子晶体的结构演化
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2022-08-07 , DOI: 10.1002/adfm.202203894
Kun Ni ₁ , Fei Pan ₁ , Yanwu Zhu ₁

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在过去的几十年里，富勒烯和多种衍生物的制备备受关注。了解从富勒烯开始的结构演变对于指导实验探索至关重要，但尚未受到关注。使用从头算分子动力学或全局结构搜索算法结合密度泛函理论计算可以一目了然的势能面（PES），但成本高，效率低。在此，通过使用神经网络势和随机表面行走全局结构搜索方法，加速能量计算，以及从 C _{60开始的更高效的 PES 映射}报道了分子晶体。发现结构演化遵循分子晶体→聚合物→打开的笼有序结构→3D）在零压力下弯曲的碳和石墨的顺序。在高压下，例如50 GPa，演化遵循富勒烯→sp ²和sp ³杂化碳→sp ³无定形碳和晶体金刚石的路径。在演化路径中获得的结构的电子性质计算显示带隙取决于生成的结构的有序参数，这表明可以在实验中制备更多新型碳，从 C ₆₀开始。

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Structural Evolution of C60 Molecular Crystal Predicted by Neural Network Potential

The preparation of fullerene and a wide range of derivatives has attracted much attention in past decades. Understanding the structural evolution starting from fullerene is critical to guide the experimental exploration but has been paid less attention yet. Using ab initio molecular dynamics or global structural search algorithm accompanied with density functional theory calculations can give a glance of the potential energy surface (PES), but suffers high cost and low efficiency. Herein, by using neural network potentials and stochastic surface walking global structural search method, an accelerated energy calculation, and the higher efficient PES mapping starting from C₆₀ molecular crystal are reported. The structural evolution is found to follow an order of molecular crystal → polymers → opened caged ordered structures → 3D) curved carbon and graphite under zero pressure. Under high pressures, e.g., 50 GPa, the evolution follows a pathway of fullerene → sp² and sp³ hybrid carbon → sp³ amorphous carbon and crystal diamond. The electronic property calculation of the obtained structures in the evolution pathway shows a band gap depending on the order parameter of the generated structures, suggesting that more novel carbons can be potentially prepared in experiments, starting from C₆₀.

更新日期：2022-08-07

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