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Journal of Nanoelectronics and Optoelectronics

"Dark" and "Bright" Excitons in Carbon Nanotubes: New Media for Quantum Optics

Nikolai G. Kalugin, Yuri V. Rostovtsev

Published May 24, 2010• 4 citations
Publisher

Abstract

It is well-known that strong Coulomb effects in carbon nanotubes lead to formation of the so-called bright and (forbidden one-photon optical transition) exciton states, and dramatically decrease the efficiency of one-photon light emission via trapping of the carriers by states. We suggest and demonstrate that the proper use of these bright and exciton states with distinctively different recombination times may turn the situation around: the use of quantum coherence and multiphoton schemes of excitation potentially not only allow one to efficiently manipulate the dark states, but can also create conditions for efficient light generation in different frequency regions, produce slow or fast light, implement quantum light storage, and media with a negative refractive index. We discuss possible applications of the quantum coherent effects to quantum-optical carbon nanotube devices that have a potential for suitable performance at elevated temperatures, because the binding energies of excitons in single-walled nanotubes are hundreds-of-meV high.

DOI
10.1166/jno.2009.1043

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It is well-known that strong Coulomb effects in carbon nanotubes lead to formation of the so-called bright and (forbidden one-photon optical transition) exciton states, and dramatically decrease the efficiency of one-photon light emission via trapping of the carriers by states. We suggest and demonstrate that the proper use of these bright and exciton states with distinctively different recombination times may turn the situation around: the use of quantum coherence and multiphoton schemes of excitation potentially not only allow one to efficiently manipulate the dark states, but can also create conditions for efficient light generation in different frequency regions, produce slow or fast light, implement quantum light storage, and media with a negative refractive index. We discuss possible applications of the quantum coherent effects to quantum-optical carbon nanotube devices that have a potential for suitable performance at elevated temperatures, because the binding energies of excitons in single-walled nanotubes are hundreds-of-meV high.
It is strong Coulomb effects in carbon nanotubes that lead to formation of the so-called "bright" and "dark" (forbidden one-photon optical transition) exciton states, and dramatically decrease the efficiency of one-photon light emission via trapping of the carriers by "dark" states. We demonstrate that the proper use of these "bright" and "dark" exciton states with distinctively different recombination times may turn the situation around: the use of quantum coherence and multiphoton schemes of excitation potentially not only allow one to efficiently manipulate the dark states, but can also create conditions for efficient light generation in different frequency regions, produce "slow" or "fast" light, implement quantum light storage, media with a negative refractive index, and other quantum-optical regimes. Possible quantum-optical carbon nanotube devices have a potential for suitable performance at elevated temperatures, because the binding energies of excitons in single-walled nanotubes are hundreds-of-meV high.
We study quantum optical properties of the single-walled carbon nanotube (SWCNT) by introducing the effective interaction between the quantized electromagnetic field and the confined electrons in the SWCNT. Our purpose is to explore the quantum natures of electron transport in the SWCNT by probing its various quantum optical properties relevant to quantum coherence, such as the interference of the scattered and emitted photons, and the bunching and anti-bunching of photons which are characterized by the higher order coherence functions. In the strong field limit, we study the interband Rabi oscillation of electrons driven by a classical light. We also investigate the possible lasing mechanism in superradiation of coherent electrons in a SWCNT driven by a light pump or electron injection, which generate electron population inversion in the higher energy-band of SWCNT.
We report the first observation of photon antibunching in the photoluminescence from single carbon nanotubes. The emergence of a fast luminescence decay component under strong optical excitation indicates that Auger processes are partially responsible for inhibiting two-photon generation. Additionally, the presence of exciton localization at low temperatures ensures that nanotubes emit photons predominantly one by one. The fact that multiphoton emission probability can be smaller than 5% suggests that carbon nanotubes could be used as a source of single photons for applications in quantum cryptography.
Quantum optics phenomena, including light absorbtion and atomic states entanglement, are discussed for carbon nanotubes doped with atoms (ions). It has been shown that, similar to semiconductor microcavities and photonic band-gap materials, carbon nanotubes may qualitatively change the character of the atom-electromagnetic-field interactions, yielding strong atom-field coupling regime with the formation of quasi-one-dimensional atomic polaritons. These may be observed experimentally via the effect of the absorption line splitting (Rabi splitting) in the frequency range close to the atomic transition frequency. A scheme for entangling atomic polaritons is investigated using the photon Green function formalism for quantizing electromagnetic fields in the presence of quasi-one-dimensional absorbing and dispersing media. Small-diameter metallic nanotubes are shown to result in sizable amounts of the two-qubit atomic entanglement with no damping for sufficiently long times, thus challenging novel applications of atomically doped carbon nanotubes in quantum information science.
Optical nonlinearities can be engineered into high-speed optical gates when a probe signal is switched coherently and fast by an optical control pulse through various nonlinear effects for switching. In semiconductors, a strong light–matter interaction can also excite many electrons to interact with each other, which can deteriorate switching through Coulomb-induced dephasing. Here, we demonstrate that optical transmission of carbon nanotubes can be switched reversibly hundreds of times via detuned Rabi splitting, faster than 200 fs via nonresonant but strong control pulses. Our detailed experiment–theory analysis identifies that quantum memory in Coulombic scattering restores reversibility while simultaneously reducing undesirable pure dephasing of coherences. This capability creates new possibilities for ultrafast quantum optoelectronic processing in quantum materials.
Carbon nanotubes (CNTs) have been studied exhaustively in terms of electronic and mechanical properties. A large repertoire of potential applications has been demonstrated for these one-dimensional systems of rolled-up sheets of carbon. To date, most of the optical studies on CNTs have focused more on characterization. Högele et al. now show that CNTs exhibit quantum optical behavior. Photons, being bosons, like to bunch together. However, in quantum systems such as atoms and artificial atoms, the confinement of carriers can split the pack behavior, resulting in the photons being emitted one at a time. For applications such as ultrasecure communication, such antibunching behavior is desirable. These authors excite a single CNT with a laser pulse and observe that light is emitted as single photons upon relaxation. The results suggest that CNTs may extend their repertoire beyond logic circuits and other electronic devices, finding application in quantum optoelectronics. — ISO