Excitonic Resonances in Coherent Anti-Stokes Raman Scattering from Single-Walled Carbon Nanotubes

In this work we investigate the role of exciton resonances in coherent anti-Stokes Raman scattering (er-CARS) in single walled carbon nanotubes (SWCNTs). We drive the nanotube system in simultaneous phonon and excitonic resonances, where we observe a superior enhancement by orders of magnitude exceeding non-resonant cases. We investigated the resonant effects in five $(n,m)$ chiralities and find that the er-CARS intensity varies drastically between different nanotube species. The experimental results are compared with a perturbation theory model. Finally, we show that such giant resonant non-linear signals enable rapid mapping and local heating of individualized CNTs, suggesting easy tracking of CNTs for future nanotoxology studies and therapeutic application in biological tissues

Excitonic Resonances in Coherent Anti-Stokes Raman Scattering from Single Wall Carbon Nanotubes

In this work we investigate the role of exciton resonances in coherent anti-Stokes Raman scattering (er-CARS) in single walled carbon nanotubes (SWCNTs). We drive the nanotube system in simultaneous phonon and excitonic resonances, where we observe a superior enhancement by orders of magnitude exceeding non-resonant cases. We investigated the resonant effects in five $(n,m)$ chiralities and find that the er-CARS intensity varies drastically between different nanotube species. The experimental results are compared with a perturbation theory model. Finally, we show that such giant resonant non-linear signals enable rapid mapping and local heating of individualized CNTs, suggesting easy tracking of CNTs for future nanotoxology studies and therapeutic application in biological tissues.Comment: 17 pages, 6 figure

Exciton decay dynamics in individual carbon nanotubes at room temperature

We studied the exciton decay dynamics of individual semiconducting single-walled carbon nanotubes at room temperature using time-resolved photoluminescence spectroscopy. The photoluminescence decay from nanotubes of the same (n,m) type follows a single exponential decay function, however, with lifetimes varying between about 1 and 40 ps from nanotube to nanotube. A correlation between broad photoluminescence spectra and short lifetimes was found and explained by defects promoting both nonradiative decay and vibronic dephasing

Visualizing the Local Optical Response of Semiconducting Carbon Nanotubes to DNA-Wrapping

We studied the local optical response of semiconducting single-walled carbon nanotubes to wrapping by DNA segments using high resolution tip-enhanced near-field microscopy. Photoluminescence (PL) near-field images of single nanotubes reveal large DNA-wrapping-induced red shifts of the exciton energy that are two times higher than indicated by spatially averaging confocal microscopy. Near-field PL spectra taken along nanotubes feature two distinct PL bands resulting from DNA-wrapped and unwrapped nanotube segments. The transition between the two energy levels occurs on a length scale smaller than our spatial resolution of about 15 nm