Abstract
Single-walled carbon nanotubes (SWNTs) are π-conjugated, quasi-one-dimensional structures consisting of rolled-up graphene sheets that, depending on their chirality, behave as semiconductors or metals1; owing to their unique properties, they enable groundbreaking applications in mechanics, nanoelectronics and photonics2,3. In semiconducting SWNTs, medium-sized excitons (3–5 nm) with large binding energy and oscillator strength are the fundamental excitations4,5,6,7,8; exciton wavefunction localization and one-dimensionality give rise to a strong electron–phonon coupling9,10,11, the study of which is crucial for the understanding of their electronic and optical properties. Here we report on the use of resonant sub-10-fs visible pulses12 to generate and detect, in the time domain, coherent phonons in SWNT ensembles. We observe vibrational wavepackets for the radial breathing mode (RBM) and the G mode, and in particular their anharmonic coupling, resulting in a frequency modulation of the G mode by the RBM. Quantum-chemical modelling13 shows that this effect is due to a corrugation of the SWNT surface on photoexcitation, leading to a coupling between longitudinal and radial vibrations.
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Acknowledgements
We thank G. Marcolongo for technical help and Z. V. Vardeny for useful discussions. M.M., G.L. and E.M. acknowledge financial support from MIUR (contracts PRIN-2004035502, FIRB-RBNE 033KMA, FIRB-RBNE01P4JF). The research at LANL is supported by the Center for Integrated Nanotechnology (CINT), Los Alamos LDRD Funds and the Office of Basic Energy Sciences, US Department of Energy. This support is gratefully acknowledged.
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Gambetta, A., Manzoni, C., Menna, E. et al. Real-time observation of nonlinear coherent phonon dynamics in single-walled carbon nanotubes. Nature Phys 2, 515–520 (2006). https://doi.org/10.1038/nphys345
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DOI: https://doi.org/10.1038/nphys345
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