Effect of oxygen and nitrogen functionalization on the physical and electronic structure of graphene

Effect of oxygen and nitrogen functionalization on the physical and electronic structure of graphene
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DOI:
10.1007/s12274-015-0768-0
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发表时间:
2015-08-01
期刊:
影响因子:
9.9
通讯作者:
Wilson, Neil R.
Wilson, Neil R.
中科院分区:
材料科学1区
文献类型:
--
作者:
Marsden, Alexander J.;Brommer, Peter;Wilson, Neil R.

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石墨烯的共价官能化提供了定制其性质的机会,并且是一些石墨烯合成技术的不可避免的结果。然而,由官能化引起的变化还没有很好地理解。通过使用原子源控制氧和氮的功能化程度,我们在原子尺度上研究了结构和性能的演变。原子氧可逆地引入环氧基团,而在类似的条件下,原子氮不可逆地产生不同的官能团,包括取代,吡啶和吡咯氮。原子氧在狄拉克点(即,未掺杂的),而原子氮导致净n掺杂;然而,实验结果与主要的电子效应一致,因为两者都是从离域态到局域态的转变,并且因此石墨烯的特征电子结构的损失。
Covalent functionalization of graphene offers opportunities for tailoring its properties and is an unavoidable consequence of some graphene synthesis techniques. However, the changes induced by the functionalization are not well understood. By using atomic sources to control the extent of the oxygen and nitrogen functionalization, we studied the evolution in the structure and properties at the atomic scale. Atomic oxygen reversibly introduces epoxide groups whilst, under similar conditions, atomic nitrogen irreversibly creates diverse functionalities including substitutional, pyridinic, and pyrrolic nitrogen. Atomic oxygen leaves the Fermi energy at the Dirac point (i.e., undoped), whilst atomic nitrogen results in a net n-doping; however, the experimental results are consistent with the dominant electronic effect for both being a transition from delocalized to localized states, and hence the loss of the signature electronic structure of graphene.