Surface Confined Hydrogenation of Graphene Nanoribbons.

Surface Confined Hydrogenation of Graphene Nanoribbons.
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DOI:
10.1021/acsnano.1c11372
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发表时间:
2022-07-26
期刊:
影响因子:
17.1
通讯作者:
Schaub, Renald
Schaub, Renald
中科院分区:
材料科学1区
文献类型:
--
作者:
Sung, Yi-Ying;Vejayan, Harmina;Baddeley, Christopher J.;V. Richardson, Neville;Grillo, Federico;Schaub, Renald

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利用设计的前驱体分子进行表面合成被认为是制备宽度确定、电子性质可调的石墨烯纳米带的有效方法。最近的报道表明,在大多数情况下,掺杂原子(如硼、氮和硫)的带隙在大小上保持不变。然而,理论预测可以通过氢化来设计可调的带隙,但到目前为止还缺乏这方面的实验证据。本文报道了在超高真空环境中生长在Au(111)表面上的7-扶手椅型石墨烯纳米带(7-AGNRs)的表面受限氢化研究。GNR首先被制备,然后通过暴露在活化的氢原子中进行氢化。高分辨电子能量损失谱(HREELS)和扫描隧道显微镜(STM)图像揭示了一个自限氢化过程。结合键分辨扫描隧道显微镜(BRSTM)成像和针尖诱导定点脱氢,详细研究了氢化机理,并用密度泛函理论(DFT)计算方法对实验结果进行了补充。结果表明,在所有情况下,GnR/Au(111)体系都成功地通过边和基面氢化改变了体系的电子性质,并提出了氢化过程的机理。
On-surface synthesis with designer precursor molecules is considered an effective method for preparing graphene nanoribbons (GNRs) of well-defined widths and with tunable electronic properties. Recent reports have shown that the band gap of ribbons doped with heteroatoms (such as boron, nitrogen, and sulfur) remains unchanged in magnitude in most cases. Nevertheless, theory predicts that a tunable band gap may be engineered by hydrogenation, but experimental evidence for this is so far lacking. Herein, surface-confined hydrogenation studies of 7-armchair graphene nanoribbons (7-AGNRs) grown on Au(111) surfaces, in an ultrahigh vacuum environment, are reported. GNRs are first prepared, then hydrogenated by exposure to activated hydrogen atoms. High resolution electron energy loss spectroscopy (HREELS) and scanning tunneling microscopy (STM) images reveal a self-limited hydrogenation process. By means of a combination of bond-resolved scanning tunneling microscopy (BRSTM) imaging and tip-induced site-specific dehydrogenation, the hydrogenation mechanism is studied in detail, and density-functional theory (DFT) calculation methods are used to complement the experimental findings. In all cases, the results demonstrate the successful modification of the electronic properties of the GNR/Au(111) system by edge and basal-plane hydrogenation, and a mechanism for the hydrogenation process is proposed.
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