Real-time ab initio simulations of excited carrier dynamics in carbon nanotubes.

Combining time-dependent density functional calculations for electrons with molecular dynamics simulations for ions, we investigate the dynamics of excited carriers in a (3,3) carbon nanotube at different temperatures. Following an hnu=6.8 eV photoexcitation, the carrier decay is initially dominated by efficient coupling to electronic degrees of freedom. At room temperature, the excitation gap is reduced to nearly half its initial value after approximately 230 fs, where coupling to ionic motion starts dominating the decay. We show that the onset point and damping rate in the phonon regime change with initial ion velocities, a manifestation of temperature-dependent coupling between electronic and ionic degrees of freedom.