Ultrafast generation of fundamental and multiple-order phonon excitations in highly enriched (6,5) single-wall carbon...

Using a macroscopic ensemble of highly enriched (6,5) single-wall carbon nanotubes, combined with high signal-to-noise ratio and time-dependent differential transmission spectroscopy, we have generated vibrational modes in an ultrawide spectral range (10-3000 cm(-1)). A total of 14 modes were clearly resolved and identified, including fundamental modes of A, E1, and E2 symmetries and their combinational modes involving two and three phonons. Through comparison with continuous wave Raman spectra as well as calculations based on an extended tight-binding model, we were able to identify all the observed peaks and determine the frequencies of the individual and combined modes. We provide a full summary of phonon frequencies for (6,5) nanotubes that can serve as a basic reference with which to refine our understanding of nanotube phonon spectra as well as a testbed for new theoretical models.