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Covalent bonding interactions determine the energy–momentum (E–k) dispersion (band structure) of solid-state materials. Here, we show that noncovalent interactions can modulate theE–kdispersion 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. 

Semiconducting carbon nanotubes are robust molecules with nanometer-scale diameters that can be used in field-effect transistors, from larger thin-film implementation to devices that work in conjunction with silicon electronics, and can potentially be used as a platform for high-performance digital electronics as well as radio-frequency and sensing applications. Recent progress in the materials, devices, and technologies related to carbon nanotube transistors is briefly reviewed. Emphasis is placed on the most broadly impactful advancements that have evolved from single-nanotube devices to implementations with aligned nanotubes and even nanotube thin films. There are obstacles that remain to be addressed, including material synthesis and processing control, device structure design and transport considerations, and further integration demonstrations with improved reproducibility and reliability; however, the integration of more than 10,000 devices in single functional chips has already been realized.