A Kinetic Pathway toward High-Density Ordered N Doping of Epitaxial Graphene on Cu(111) Using C5NCl5 Precursors
A Kinetic Pathway toward High-Density Ordered N Doping of Epitaxial Graphene on Cu(111) Using C5NCl5 Precursors
复制标题
使用 C5NCl5 前驱体在 Cu(111) 上进行高密度有序 N 外延石墨烯掺杂的动力学途径
DOI：
10.1021/jacs.6b12506
复制
发表时间：
2017-05-31
影响因子：
15
通讯作者：
Zhang, Zhenyu
中科院分区：
文献类型：
--
作者：
Cui, Ping;Choi, Jin-Ho;Zhang, Zhenyu
原始石墨烯具有高的电迁移率，但其低载流子密度严重限制了其技术意义。过去通过化学掺杂来增加石墨烯载流子密度的努力已经显示出有限的成功，伴随着由无序掺杂剂引起的迁移率的大幅降低。在这里，基于第一性原理计算，我们建议通过C5 NCl 5分子前体的自组装在Cu（111）上生长石墨烯，以实现高密度（1/6）和高度有序的氮掺杂。这样一个过程依赖于优雅的协同作用所发挥的伦敦分散，化学和筛选库仑排斥力，在增强分子吸附，促进容易脱氯，并支配的C5 N自由基的整体方向，分别。从取向相关的石墨烯岛的进一步生长伴随着显著最小化的晶界密度，因为晶粒聚结以形成更大的N掺杂的石墨烯片，其进一步显示出具有用于未来器件应用的优异的电子特性。还研究了使用C5 NH 5前体生长N掺杂石墨烯的初始动力学过程，并与C5 NCl 5进行了对比。
Pristine graphene possesses high electrical mobility, but its low charge carrier density severely limits its technological significance. Past efforts to increase graphenes carrier density via chemical doping have shown limited successes, accompanied by substantial reductions in the mobility caused by disordered dopants. Here, based on first-principles calculations, we propose to grow graphene on Cu(111) via self-assembly of C5NCl5 molecular precursors to achieve high-density (1/6) and highly ordered nitrogen doping. Such a process relies on the elegant concerted roles played by the London dispersion, chemical, and screened Coulomb repulsive forces in enhancing molecular adsorption, facilitating easy dechlorination, and dictating the overall orientation of the C5N radicals, respectively. Further growth from the orientationally correlated graphene islands is accompanied by significantly minimized density of grain boundaries as the grains coalesce to form larger N-doped graphene sheets, which are further shown to possess superb electronic properties for future device applications. Initial kinetic processes involved in N-doped graphene growth using C5NH5 precursors are also investigated and contrasted with that of C5NCl5.