Chiral selective reactivity and redox chemistry of carbon nanotubes are two emerging fields of nanoscience. These areas hold strong promise for producing methods for isolating nanotubes into pure samples of a single electronic type, and for reversible doping of nanotubes for electronics applications. Here, we study the selective reactivity of single-walled carbon nanotubes with organic acceptor molecules. We observe spectral bleaching of the nanotube electronic transitions consistent with an electron-transfer reaction occurring from the nanotubes to the organic acceptors. The reaction kinetics are found to have a strong chiral dependence, with rates being slowest for large-bandgap species and increasing for smaller-bandgap nanotubes. The chiral-dependent kinetics can be tuned to effectively freeze the reacted spectra at a fixed chiral distribution. Such tunable redox chemistry may be important for future applications in reversible non-covalent modification of nanotube electronic properties and in chiral selective separations.
We have studied the optical transition energies of single-wall carbon nanotubes over broad diameter (0.7-2.3 nm) and energy (1.26-2.71 eV) ranges, using their radial breathing mode Raman spectra. We establish the diameter and chiral angle dependence of the poorly studied third and fourth optical transitions in semiconducting tubes. Comparative analysis between the higher lying transitions and the first and second transitions show two different diameter scalings. Quantum mechanical calculations explain the result showing strongly bound excitons in the first and second transitions and a delocalized electron wave function in the third transition.
Since the discovery of carbon nanotubes in 1991 by Iijima, there has been great interest in creating long, continuous nanotubes for applications where their properties coupled with extended lengths will enable new technology developments. For example, ultralong nanotubes can be spun into fibres that are more than an order of magnitude stronger than any current structural material, allowing revolutionary advances in lightweight, high-strength applications. Long metallic nanotubes will enable new types of micro-electromechanical systems such as micro-electric motors, and can also act as a nanoconducting cable for wiring micro-electronic devices. Here we report the synthesis of 4-cm-long individual single-wall carbon nanotubes (SWNTs) at a high growth rate of 11 microm s(-1) by catalytic chemical vapour deposition. Our results suggest the possibility of growing SWNTs continuously without any apparent length limitation.
Improved electron transport along a carbon nanotube (CNT) fiber when it is spun from an array of longer nanotubes is reported. The effect of chemical post‐treatments is also demonstrated. For example, the covalent bonding of gold nanoparticles to the CNT fibers remarkably improves conductivity (see figure), whereas annealing CNT fibers in a hydrogen‐containing atmosphere leads to a dramatic decrease in conductivity.
On-demand single-photon sources capable of operating at room temperature and the telecom wavelength range of 1,300-1,500 nm hold the key to the realization of novel technologies that span from sub-diffraction imaging to quantum key distribution and photonic quantum information processing. Here, we show that incorporation of undoped (6,5) single-walled carbon nanotubes into a SiO2 matrix can lead to the creation of solitary oxygen dopant states capable of fluctuation-free, room-temperature single-photon emission in the 1,100-1,300 nm wavelength range. We investigated the effects of temperature on photoluminescence emission efficiencies, fluctuations and decay dynamics of the dopant states and determined the conditions most suitable for the observation of single-photon emission. This emission can in principle be extended to 1,500 nm by doping of smaller-bandgap single-walled carbon nanotubes. This easy tunability presents a distinct advantage over existing defect centre single-photon emitters (for example, diamond defect centres). Our SiO2-encapsulated sample also presents exciting opportunities to apply Si/SiO2-based micro/nano-device fabrication techniques in the development of electrically driven single-photon sources and integration of these sources into quantum photonic devices and networks.
Cycloparaphenylenes, the simplest structural unit of armchair carbon nanotubes, have unique optoelectronic properties counterintuitive in the class of conjugated organic materials. Our time-dependent density functional theory study and excited state dynamics simulations of cycloparaphenylene chromophores provide a simple and conceptually appealing physical picture explaining experimentally observed trends in optical properties in this family of molecules. Fully delocalized degenerate second and third excitonic states define linear absorption spectra. Self-trapping of the lowest excitonic state due to electron−phonon coupling leads to the formation of spatially localized excitation in large cycloparaphenylenes within 100 fs. This invalidates the commonly used Condon approximation and breaks optical selection rules, making these materials superior fluorophores. This process does not occur in the small molecules, which remain inefficient emitters. A complex interplay of symmetry, π-conjugation, conformational distortion and bending strain controls all photophysics of cycloparaphenylenes.
Progress in quantum computing and quantum cryptography requires efficient, electrically triggered, single-photon sources at room temperature in the telecom wavelengths. It has been long known that semiconducting single-wall carbon nanotubes (SWCNTs) display strong excitonic binding and emit light over a broad range of wavelengths, but their use has been hampered by a low quantum yield and a high sensitivity to spectral diffusion and blinking. In this Perspective, we discuss recent advances in the mastering of SWCNT optical properties by chemistry, electrical contacting and resonator coupling towards advancing their use as quantum light sources. We describe the latest results in terms of single-photon purity, generation efficiency and indistinguishability. Finally, we consider the main fundamental challenges stemming from the unique properties of SWCNTs and the most promising roads for SWCNT-based chip integrated quantum photonic sources.
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