Fermi-Level Engineering of Nitrogen Core-Doped Armchair Graphene Nanoribbons.
Fermi-Level Engineering of Nitrogen Core-Doped Armchair Graphene Nanoribbons.
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DOI：
10.1021/jacs.3c05755
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发表时间：
2023-09-06
影响因子：
15
通讯作者：
Fischer, Felix R.
中科院分区：
文献类型：
--
作者：
Wen, Ethan Chi Ho;Jacobse, Peter H.;Jiang, Jingwei;Wang, Ziyi;Louie, Steven G.;Crommie, Michael F.;Fischer, Felix R.
自下而上设计的一维石墨烯纳米带(GNRs)替代杂原子掺杂是实现纳米电子学和传感低维功能材料的通用工具。以前的努力在很大程度上依赖于用三角平面N原子取代排列在GNR边缘的C-H基团。然而，这种原子精确的掺杂只导致价带(Vb)和导带(CB)能量的适度重新排列。在这里，我们报道了氮核掺杂的5原子宽扶手椅GNRs(N2-5-AGNRs)的设计、自下而上的合成和光谱表征，它产生了更大的GNR电子结构能级位移。在这里，沿着GNR主干用N原子取代C原子，在每个掺杂剂中引入一个过剩的π电子，该电子填充与先前未被占据的能带相关联的电子态。第一性原理密度泛函理论计算证实，费米能量的显著变化(∼1.0 eV)伴随着能带结构的广泛重新配置，包括新带隙的打开和从直接半导体带隙到间接半导体带隙的转变。扫描隧道谱(STS)剥离电荷输运实验证实了理论结果，揭示了这种新型N掺杂GNR的代位杂原子掺杂、费米能级移动、电子能带结构和拓扑工程之间的关系。
Substitutional heteroatom doping of bottom-up engineered 1D graphene nanoribbons (GNRs) is a versatile tool for realizing low-dimensional functional materials for nanoelectronics and sensing. Previous efforts have largely relied on replacing C–H groups lining the edges of GNRs with trigonal planar N atoms. This type of atomically precise doping, however, only results in a modest realignment of the valence band (VB) and conduction band (CB) energies. Here, we report the design, bottom-up synthesis, and spectroscopic characterization of nitrogen core-doped 5-atom-wide armchair GNRs (N2-5-AGNRs) that yield much greater energy-level shifting of the GNR electronic structure. Here, the substitution of C atoms with N atoms along the backbone of the GNR introduces a single surplus π-electron per dopant that populates the electronic states associated with previously unoccupied bands. First-principles DFT-LDA calculations confirm that a sizable shift in Fermi energy (∼1.0 eV) is accompanied by a broad reconfiguration of the band structure, including the opening of a new band gap and the transition from a direct to an indirect semiconducting band gap. Scanning tunneling spectroscopy (STS) lift-off charge transport experiments corroborate the theoretical results and reveal the relationship among substitutional heteroatom doping, Fermi-level shifting, electronic band structure, and topological engineering for this new N-doped GNR.
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四元环石墨烯纳米带中的赝原子轨道行为。
影响因子：
13.6
作者：
Jacobse PH;Jin Z;Jiang J;Peurifoy S;Yue Z;Wang Z;Rizzo DJ;Louie SG;Nuckolls C;Crommie MF
通讯作者：
Crommie MF
影响因子：
17.1
作者：
Li, Jingcheng;Brandimarte, Pedro;Ignacio Pascual, Jose
通讯作者：
Ignacio Pascual, Jose
影响因子：
4.3
作者：
Marangoni, Tomas;Haberer, Danny;Fischer, Felix R.
通讯作者：
Fischer, Felix R.
影响因子：
3.7
作者：
Frank, Sebastian;Jacob, David
通讯作者：
Jacob, David
影响因子：
17.1
作者：
Lawrence, James;Brandimarte, Pedro;de Oteyza, Dimas G.
通讯作者：
de Oteyza, Dimas G.