Dephasing of G-Band Phonons in Single-Wall Carbon Nanotubes Probed via Impulsive Stimulated Raman Scattering

We have studied the coherent dynamics of G-band phonons in single-walled carbon nanotubes through impulsive stimulated Stokes and anti-Stokes Raman scattering. The probe energy dependence of phonon amplitude as well as preferential occurrence between Stokes and anti-Stokes components in response to chirped-pulse excitation are well explained within our model. The temperature dependence of the observed dephasing rate clearly exhibits a thermally-activated component, with an activation energy that coincides with the frequency of the radial breathing mode (RBM). This fact provides a clear picture for the dephasing of optical phonons by random frequency modulation via interaction with the RBM through anharmonicity.

Resonant Coherent Phonon Generation in Single-Walled Carbon Nanotubes through Near-Band-Edge Excitation

We have observed large-amplitude coherent phonon oscillations of radial breathing modes (RBMs) in single-walled carbon nanotubes excited through the lowest-energy (E11) interband transitions. In contrast to the previously-studied coherent phonons excited through higher-energy (E22) transitions, these RBMs show comparable intensities between (n-m) mod 3 = 1 and -1 nanotubes. We also find novel non-resonantly excited RBMs over an excitation range of ~300 meV above the E11 transition, which we attribute to multi-phonon replicas arising from strong exciton-phonon coupling.