We have studied ultrafast spectral diffusion (SD) within exciton bands of semiconducting single-wall carbon nanotubes (s-SWNTs) using one-and two-dimensional, near-infrared transient hole burning spectroscopy and time-resolved fluorescence spectroscopy at temperatures between 15 K and 293 K. We find that inhomogeneous spectral broadening of 60 meV for s-SWNTs embedded in gelatin exceeds the homogeneous linewidth of 3.3 meV by over an order of magnitude. The experiments show that ultrafast spectral diffusion of excitons in gel-immobilized s-SWNTs on the 250 fs time-scale can be attributed to axial intra-tube exciton diffusion. Comparison with kinetic Monte Carlo simulations suggests that the length-scale characteristic of the granularity of the axial potential energy landscape is about 24 nm.
Doping can profoundly affect the electronicand optical-structure of semiconductors. Here we address the effect of surplus charges on nonradiative (NR) exciton and trion decay in doped semiconducting single-wall carbon nanotubes. The dependence of exciton photoluminescence quantum yields and exciton decay on the doping level, with its characteristically stretchedexponential kinetics, is attributed to diffusionlimited NR decay at charged impurity sites. By contrast, trion decay is unimolecular with a rate constant of 2.0 ps −1 . Our experiments thus show that charged impurities not only trap trions and scavenge mobile excitons but that they also facilitate efficient NR energy dissipation for both.
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