Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Physical Review B

Dephasing in semiconducting single-walled carbon nanotubes induced by exciton-exciton annihilation

Darius Abramavičius, Ying‐Zhong Ma, Matt W. Graham, Leonas Valkūnas, Graham R. Fleming

Published May 29, 2009• 26 citations
Publisher

Abstract

Three-pulse photon echo peak-shift measurements were performed on semiconducting single-walled carbon nanotubes embedded in a polymer matrix at room temperature. We found a striking dependence of the peak shift on the excitation intensity. Numerical simulations based on an interacting-boson model demonstrate that the intensity dependence originates from a highly nonlinear optical response initiated by exciton-exciton annihilation.

DOI
10.1103/physrevb.79.195445

Related papers

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

Nikolai G. Kalugin, Yuri V. Rostovtsev

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.

Journal of Nanoelectronics and Optoelectronics•May 24, 2010•4 citations

Three-pulse photon echo of an excitonic dimer modeled via Redfield theory

Pär Kjellberg, Tõnu Pullerits

In this article the third-order response of an excitonically coupled dimer is studied. The three-pulse photon echo signals were calculated by extracting polarization components from the total polarization in the corresponding phase-matched directions. The total nonlinear response was obtained by numeric propagation of the density matrix, with the exciton-vibrational coupling modeled via Redfield relaxation theory. The full two-dimensional three-pulse photon echo signals and the peak shift were analyzed in terms of the density-matrix dynamics of coherence dephasing and population relaxation. The location of the two-exciton state was found to be essential for proper modeling of the three-pulse photon echo. In particular, an oscillation in the three-pulse photon echo peak shift is found if the two-exciton state is displaced. The oscillations can be related to the dynamics of the one-exciton coherences.

The Journal of Chemical Physics•Jan 6, 2006•35 citations

"Dark" vs "Bright" Excitons in Carbon Nanotubes: Applications to Quantum Optics

Nikolai G. Kalugin, Yuri V. Rostovtsev

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.

arXiv:0902.1163•Feb 6, 2009•1 citation

Room-Temperature Single-Photon Emission from Micrometer-Long Air-Suspended Carbon Nanotubes

A. Ishii, T. Uda, Y. K. Kato

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.

arXiv:1707.05435•Physical Review Applied•Nov 20, 2017•43 citations

Photon Antibunching in the Photoluminescence Spectra of a Single Carbon Nanotube

Alexander Högele, Christophe Galland, Martin Winger +1 more

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.

arXiv:0707.1923•Physical Review Letters•May 27, 2008•274 citations

Nonlinear Response of Localized Excitons: Effects of the Excitation-Induced Dephasing

Paola Borri, W. Langbein, D. Birkedal +2 more

The polarization dependence of the ultrafast nonlinear response of localized excitons in GaAs/AlGaAs quantum wells has been investigated by spectrally resolved, transient four-wave mixing. The role of the excitation-induced dephasing in the delay dependence of the signal is discussed in detail. In particular, we show experimentally that the excitation-induced dephasing gives rise to a photon echo in inhomogeneous systems. We develop a simple analytical model for the delay dependence of the signal, which enables us to deduce the dephasing time from the four-wave mixing decay.

physica status solidi (a)•Nov 1, 1997•8 citations
Three-pulse photon echo peak-shift measurements were performed on semiconducting single-walled carbon nanotubes embedded in a polymer matrix at room temperature. We found a striking dependence of the peak shift on the excitation intensity. Numerical simulations based on an interacting-boson model demonstrate that the intensity dependence originates from a highly nonlinear optical response initiated by exciton-exciton annihilation.
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.
In this article the third-order response of an excitonically coupled dimer is studied. The three-pulse photon echo signals were calculated by extracting polarization components from the total polarization in the corresponding phase-matched directions. The total nonlinear response was obtained by numeric propagation of the density matrix, with the exciton-vibrational coupling modeled via Redfield relaxation theory. The full two-dimensional three-pulse photon echo signals and the peak shift were analyzed in terms of the density-matrix dynamics of coherence dephasing and population relaxation. The location of the two-exciton state was found to be essential for proper modeling of the three-pulse photon echo. In particular, an oscillation in the three-pulse photon echo peak shift is found if the two-exciton state is displaced. The oscillations can be related to the dynamics of the one-exciton coherences.
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.
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.
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.
The polarization dependence of the ultrafast nonlinear response of localized excitons in GaAs/AlGaAs quantum wells has been investigated by spectrally resolved, transient four-wave mixing. The role of the excitation-induced dephasing in the delay dependence of the signal is discussed in detail. In particular, we show experimentally that the excitation-induced dephasing gives rise to a photon echo in inhomogeneous systems. We develop a simple analytical model for the delay dependence of the signal, which enables us to deduce the dephasing time from the four-wave mixing decay.