解决富勒烯形成之谜的多尺度模拟策略
Multiscale modeling strategy to solve fullerene formation mystery
摘要：
由于富勒烯的形成是在不可能直接观察原子级反应的条件下发生的，因此建模是揭示原子机制的唯一途径，该机制可以导致选择丰富的富勒烯异构体（如C60-Ih）。在本文中，我们回顾了不同的原子机制，通过各种建模技术所获得的结果。虽然看起来与奇数富勒烯有关的原子尺度过程（例如通过连续插入单个碳原子的生长和由额外sp原子促进的sp $^2$结构的重排）为选择丰富的异构体提供了主要贡献，但目前还没有任何决定性的证据支持任何特定的原子机制。因此，以下多尺度建模策略，以解决丰富的富勒烯异构体的高产率的奥秘建议。一方面，富勒烯异构体之间的反应可以用理论图技术来描述。另一方面，反应方案可以通过经典的分子动力学模拟与随后的从头计算的活化势垒的细化。基于这样得到的反应概率的反应集，丰富的富勒烯异构体选择的不同原子机制可以通过动力学模型进行比较。
英文摘要：
Since fullerene formation occurs under conditions where direct observation of atomic-scale reactions is not possible, modeling is the only way to reveal atomistic mechanisms which can lead to selection of abundant fullerene isomers (like C60-Ih). In the present paper we review the results obtained for different atomistic mechanisms by various modeling techniques. Although it seems that atomic-scale processes related to odd fullerenes (such as growth by consecutive insertions of single carbon atoms and rearrangements of the sp$^2$ structure promoted by extra sp atoms) provide the main contribution to selection of abundant isomers, at the moment there is no conclusive evidence in favor of any particular atomistic mechanism. Thus, the following multiscale modeling strategy to solve the mystery of the high yield of abundant fullerene isomers is suggested. On the one hand, sets of reactions between fullerene isomers can be described using theoretical graph techniques. On the other hand, reaction schemes can be revealed by classical molecular dynamics simulations with subsequent refinement of the activation barriers by ab initio calculations. Based on the reaction sets with the reaction probabilities derived in this way, the different atomistic mechanisms of abundant fullerene isomer selection can be compared by kinetic models.
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