论文标题
量子隧道驱动的h $ _2 $在石墨烯上
Quantum tunnelling driven H$_2$ formation on graphene
论文作者
论文摘要
人们普遍认为,在碳质表面上吸附的H原子在没有事件H原子的帮助下形成H $ _2 $是不利的。使用环聚合物激体理论来描述多维隧道效应,结合从头算电子结构计算,我们发现这些量子力学模拟揭示了质量不同的图像。通过深隧穿的较高的隧道,据信在低温下在低温下无关的吸附H原子的重组,反应速率通过数十个数量级提高。此外,我们确定了通过多维隧道进行H的H重组的新途径,但是可以通过对反应的简单一维描述来预测将是不可行的。结果表明,低温下的氢分子形成是相当快的过程,在实验环境和使用石墨烯,石墨和其他平面碳段的自然环境中,不应忽略它们。
It is commonly believed that it is unfavourable for adsorbed H atoms on carbonaceous surfaces to form H$_2$ without the help of incident H atoms. Using ring-polymer instanton theory to describe multidimensional tunnelling effects, combined with ab initio electronic structure calculations, we find that these quantum-mechanical simulations reveal a qualitatively different picture. Recombination of adsorbed H atoms, which was believed to be irrelevant at low temperature due to high barriers, is enabled by deep tunnelling, with reaction rates enhanced by tens of orders of magnitude. Furthermore, we identify a new path for H recombination that proceeds via multidimensional tunnelling, but would have been predicted to be unfeasible by a simple one-dimensional description of the reaction. The results suggest that hydrogen molecule formation at low temperatures are rather fast processes that should not be ignored in experimental settings and natural environments with graphene, graphite and other planar carbon segments.