Prolonged spontaneous emission and dephasing of localized excitons in air-bridged carbon nanotubes

Abstract

The bright exciton emission of semiconducting carbon nanotubes is appealing for optoelectronic and quantum photonic devices as well as fundamental studies of light-matter interaction in one-dimensional nanostructures. The photophysics of excitons in carbon nanotubes till date is however largely affected by extrinsic effects of the dielectric environment. Here we carried out time-resolved photoluminescence measurements over 14 orders of magnitude for ultra-clean carbon nanotubes bridging an airgap over pillar posts. Our measurements demonstrate a new regime of intrinsic exciton photophysics with prolonged spontaneous emission times up to T1=18 ns, between one to two orders of magnitude better than prior measurements and in agreement with values first hypothesized by theorists about a decade ago. Further we establish for the first time the exciton decoherence times of individual nanotubes in the time-domain and found four-fold prolonged values up to T2=2.1 ps compared to ensemble measurements. These first observations motivate new discussions about the magnitude of the intrinsic dephasing mechanism while the prolonged exciton dynamics is promising for device applications.

References in corpus (9)

• Coupling of Spin and Orbital Motion of Electrons in Carbon Nanotubes
• Scaling of Resistance and Electron Mean Free Path of Single-Walled Carbon Nanotubes
• Photon Antibunching in the Photoluminescence Spectra of a Single Carbon Nanotube
• Exciton energy transfer in nanotube bundles
• Structure-Dependent Fluorescence Efficiencies of Individual Single-Walled Carbon Nanotubes
• Subnanosecond spectral diffusion measurement using photon correlation
• Phonon and Electronic Non-radiative Decay of Excitons in Carbon Nanotubes
• Non-Markovian decoherence of localized nanotube excitons by acoustic phonons
• Temperature dependence of exciton recombination in semiconducting single-wall carbon nanotubes

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• Near-unity radiative quantum efficiency of excitons in carbon nanotubes
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• Near-Intrinsic Photo- and Electroluminescence from Single-Walled Carbon Nanotube Thin Films on BCB-Passivated Surfaces
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