Widely Tunable Single-Photon Source from a Carbon Nanotube in the Purcell Regime.

The narrow emission of a single carbon nanotube at low temperature is coupled to the optical mode of a fiber microcavity using the built-in spatial and spectral matching brought by this flexible geometry. A thorough cw and time-resolved investigation of the very same emitter both in free space and in cavity shows an efficient funneling of the emission into the cavity mode together with a strong emission enhancement corresponding to a Purcell factor of up to 5. At the same time, the emitted photons retain a strong sub-Poissonian statistics. By exploiting the cavity feeding effect on the phonon wings, we locked the emission of the nanotube at the cavity resonance frequency, which allowed us to tune the frequency over a 4 THz band while keeping an almost perfect antibunching. By choosing the nanotube diameter appropriately, this study paves the way to the development of carbon-based tunable single-photon sources in the telecom bands.

Diameter-selective non-covalent functionalization of carbon nanotubes with porphyrin monomers.

We report on the spontaneous non-covalent functionalization of carbon nanotubes with hydrophobic porphyrin molecules in micellar aqueous solution. By monitoring the species concentrations with optical spectroscopies, we can follow the kinetics of the reaction and study its thermodynamical equilibrium as a function of the reagent concentrations. We show that the reaction is well accounted for by a cooperative Hill equation, reaching a molecular coverage close to a compact monolayer for a porphyrin concentration larger than a diameter-specific threshold concentration. The equilibrium constant is measured for 16 nanotube chiral species. The Gibbs energy of the reaction (of the order of -40 kJ mol(-1)) and its evolution with the nanotube diameter is consistent with theoretical calculations of the binding energy. This thermodynamical study shows a strong preferential binding of TPP molecules to larger diameter nanotubes. This original curvature selectivity can be used to induce diameter selective species enrichment.

Unifying the low-temperature photoluminescence spectra of carbon nanotubes: the role of acoustic phonon confinement.

At low temperature the photoluminescence of single-wall carbon nanotubes show a large variety of spectral profiles ranging from ultranarrow lines in suspended nanotubes to broad and asymmetrical line shapes that puzzle the current interpretation in terms of exciton-phonon coupling. Here, we present a complete set of photoluminescence profiles in matrix embedded nanotubes including unprecedented narrow emission lines. We demonstrate that the diversity of the low-temperature luminescence profiles in nanotubes originates in tiny modifications of their low-energy acoustic phonon modes. When low-energy modes are locally suppressed, a sharp photoluminescence line as narrow as 0.7 meV is restored. Furthermore, multipeak luminescence profiles with specific temperature dependence show the presence of confined phonon modes.

Optically gated resonant emission of single quantum dots.

We report on the resonant emission in coherently driven single semiconductor quantum dots. We demonstrate that an ultraweak nonresonant laser acts as an optical gate for the quantum dot resonant response. We show that the gate laser suppresses Coulomb blockade at the origin of a resonant emission quenching, and that the optically gated quantum dots systematically behave as ideal two-level systems in both regimes of coherent and incoherent resonant emission.

Elastic exciton-exciton scattering in photoexcited carbon nanotubes.

We report on original nonlinear spectral hole-burning experiments in single wall carbon nanotubes that bring evidence of pure dephasing induced by exciton-exciton scattering. We show that the collision-induced broadening in carbon nanotubes is controlled by exciton-exciton scattering as for Wannier excitons in inorganic semiconductors, while the population relaxation is driven by exciton-exciton annihilation as for Frenkel excitons in organic materials. We demonstrate that this singular behavior originates from the intrinsic one-dimensionality of excitons in carbon nanotubes, which display unique hybrid features of organic and inorganic systems.

Parametric oscillation in vertical triple microcavities.

Optical parametric oscillation is a nonlinear process that enables coherent generation of 'signal' and 'idler' waves, shifted in frequency from the pump wave. Efficient parametric conversion is the paradigm for the generation of twin or entangled photons for quantum optics applications such as quantum cryptography, or for the generation of new frequencies in spectral domains not accessible by existing devices. Rapid development in the field of quantum information requires monolithic, alignment-free sources that enable efficient coupling into optical fibres and possibly electrical injection. During the past decade, much effort has been devoted to the development of integrated devices for quantum information and to the realization of all-semiconductor parametric oscillators. Nevertheless, at present optical parametric oscillators typically rely on nonlinear crystals placed into complex external cavities, and pumped by powerful external lasers. Long interaction lengths are typically required and the phase mismatch between the parametric waves propagating at different velocities results in poor parametric conversion efficiencies. Here we report the demonstration of parametric oscillation in a monolithic semiconductor triple microcavity with signal, pump and idler waves propagating along the vertical direction of the nanostructure. Alternatively, signal and idler beams can also be collected at finite angles, allowing the generation of entangled photon pairs. The pump threshold intensity is low enough to envisage the realization of an all-semiconductor electrically pumped micro-parametric oscillator.

Polariton parametric amplifier pump dynamics in the coherent regime.

We studied the pump coherent dynamics in a II-VI microcavity parametric amplifier, using angle-resolved four-wave mixing. The polariton parametric amplification is found to result in a strong quenching and saturation of the pump coherence lifetime above the threshold. For the polariton scattering processes that remain below the amplification threshold, we find an angle-dependent collision broadening associated with the efficiency of the polariton scattering towards the excitonic reservoir.

Ultrafast carrier dynamics in single-wall carbon nanotubes.

Time-resolved carrier dynamics in single-wall carbon nanotubes is investigated by means of two-color pump-probe experiments. The recombination dynamics is monitored by probing the transient photobleaching observed on the interband transitions of the semiconducting tubes. This dynamics takes place on a 1 ps time scale which is 1 order of magnitude slower than in graphite. Transient photoinduced absorption is observed for nonresonant probing and is interpreted as a global redshift of the pi-plasmon resonance. We show that the opening of the band gap in semiconducting carbon nanotubes determines the nonlinear response dynamics over the whole visible and near-infrared spectrum.