Band gap opening of metallic single-walled carbon nanotubes via noncovalent symmetry breaking.-猫眼课题宝

DOI：

10.1073/pnas.2317078121

发表时间：

2024-03

期刊：

Proceedings of the National Academy of Sciences of the United States of America

影响因子：

11.1

通讯作者：

中科院分区：

综合性期刊1区

文献类型：

作者：

Francesco Mastrocinque;George Bullard;James A Alatis;Joseph A Albro;Animesh Nayak;Nicholas X Williams;Amar Kumbhar;Hope Meikle;Zachary X W Widel;Yusong Bai;Alexis K Harvey;Joanna M Atkin;D. Waldeck;Aaron D Franklin;M. Therien

共价键相互作用决定了固态材料的能量-动量（E-k）色散（能带结构）。在这里，我们证明了非共价相互作用可以调节低维纳米尺度导体费米能级附近的E-k色散。我们证明了在金属碳纳米管表面以固定的螺旋周期包裹聚合物可以打开低能带隙。电子光谱、光斑光学、电位、电子器件和功函数数据证实，带隙打开的大小取决于聚合物电子结构的性质。聚合物解包裹逆转了导电到半导体的相变，恢复了原生金属碳纳米管的电子结构。这些结果解决了长期以来开发碳纳米管电子结构的挑战，这些结构不能通过π共轭的破坏来实现，并为设计和调谐具有数百meV带隙的专用半导体建立了路线图。

Covalent bonding interactions determine the energy-momentum (E-k) dispersion (band structure) of solid-state materials. Here, we show that noncovalent interactions can modulate the E-k dispersion near the Fermi level of a low-dimensional nanoscale conductor. We demonstrate that low energy band gaps may be opened in metallic carbon nanotubes through polymer wrapping of the nanotube surface at fixed helical periodicity. Electronic spectral, chiro-optic, potentiometric, electronic device, and work function data corroborate that the magnitude of band gap opening depends on the nature of the polymer electronic structure. Polymer dewrapping reverses the conducting-to-semiconducting phase transition, restoring the native metallic carbon nanotube electronic structure. These results address a long-standing challenge to develop carbon nanotube electronic structures that are not realized through disruption of π conjugation, and establish a roadmap for designing and tuning specialized semiconductors that feature band gaps on the order of a few hundred meV.

Band gap opening of metallic single-walled carbon nanotubes via noncovalent symmetry breaking.

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