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arXiv:0707.1923 · Physical Review Letters

Photon Antibunching in the Photoluminescence Spectra of a Single Carbon Nanotube

Alexander Högele, Christophe Galland, Martin Winger, Ataç İmamoğlu

Published May 27, 2008• 274 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1103/physrevlett.100.217401

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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.
Applications in nanophotonics and optical quantum information processing often require just one photon at a time. Although typical single-photon emitters rely on electronic states localized at the nanometer scale, the authors find that carbon nanotubes over 2 $\ensuremath{\mu}$m long exhibit photon antibunching at room temperature. Monte Carlo simulations and first-passage theory reveal that high-purity single-photon emission from this system is possible in principle, by means of efficient exciton-exciton annihilation. These results point to design strategies for single-photon sources, and provide important insight into excitonic processes in carbon nanotubes.
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.
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
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 have studied the photoluminescence correlation from a single InAs/GaAs self-assembled Stranski–Krastanow quantum dot under continuous, as well as under pulsed excitation. Under weak continuous excitation, where the single dot luminescence is due primarily to single exciton recombinations, antibunching is observed in the single dot emission correlation. Under weak pulsed excitation, the number of photons emitted by the quantum dot per pulse is close to one. We present data obtained under both conditions and are able to show that devices based on single quantum dots can be used to generate single photons.