Interdependency of subsurface carbon distribution and graphene-catalyst interaction.
Interdependency of subsurface carbon distribution and graphene-catalyst interaction.
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DOI：
10.1021/ja505454v
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发表时间：
2014-10-01
影响因子：
15
通讯作者：
Hofmann, Stephan
中科院分区：
文献类型：
--
作者：
Weatherup, Robert S.;Amara, Hakim;Blume, Raoul;Dlubak, Bruno;Bayer, Bernhard C.;Diarra, Mamadou;Bahri, Mounib;Cabrero-Vilatela, Andrea;Caneva, Sabina;Kidambi, Piran R.;Martin, Marie-Blandine;Deranlot, Cyrile;Seneor, Pierre;Schloegl, Robert;Ducastelle, Francois;Bichara, Christophe;Hofmann, Stephan
使用原位时间和深度分辨 X 射线光电子能谱以及与紧束缚模型耦合的互补正则蒙特卡罗模拟研究了化学气相沉积过程中石墨烯与催化剂相互作用的动力学。因此，我们揭示了靠近催化剂表面的碳分布与石墨烯-催化剂相互作用强度的相互依赖性。外延石墨烯与 Ni(111) 的强烈相互作用会导致催化剂表面附近溶解的碳耗尽，从而防止形成额外的层，从而导致低暴露压力（10-6-10-3 mbar）下的自限性石墨烯生长行为。碳氢化合物压力进一步增加（至〜10–1 mbar）导致石墨烯-Ni（111）相互作用减弱，并伴随着额外的石墨烯层形成，这是由近表面溶解碳浓度增加介导的。我们表明，与外延石墨烯生长的情况相比，Ni（111）上附着力较弱的旋转石墨烯的生长与最初较高水平的近表面碳有关。这些结果对石墨烯生长控制的关键影响及其与碳纳米管生长的相关性在现有文献中得到了强调。
The dynamics of the graphene–catalyst interaction during chemical vapor deposition are investigated using in situ, time- and depth-resolved X-ray photoelectron spectroscopy, and complementary grand canonical Monte Carlo simulations coupled to a tight-binding model. We thereby reveal the interdependency of the distribution of carbon close to the catalyst surface and the strength of the graphene–catalyst interaction. The strong interaction of epitaxial graphene with Ni(111) causes a depletion of dissolved carbon close to the catalyst surface, which prevents additional layer formation leading to a self-limiting graphene growth behavior for low exposure pressures (10–6–10–3 mbar). A further hydrocarbon pressure increase (to ∼10–1 mbar) leads to weakening of the graphene–Ni(111) interaction accompanied by additional graphene layer formation, mediated by an increased concentration of near-surface dissolved carbon. We show that growth of more weakly adhered, rotated graphene on Ni(111) is linked to an initially higher level of near-surface carbon compared to the case of epitaxial graphene growth. The key implications of these results for graphene growth control and their relevance to carbon nanotube growth are highlighted in the context of existing literature.
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