Femtosecond optical harmonic generation as a non-linear spectroscopic probe for carbon nanotubes

S.O. Konorov, D.A. Akimov, A.A. Ivanov, M.V. Alfimov, S. Botti, R. Ciardi, L. De Dominicis, L.S. Asilyan, A.A. Podshivalov, D.A. Sidorov-Biryukov, R. Fantoni, A.M. Zheltikov

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Second- and third-harmonic generation in single-wall carbon nanotube layers produced by low-velocity spraying was studied experimentally with the use of amplified 75 fs pulses of Cr: forsterite laser radiation within the range of pump pulse intensities up to the breakdown threshold. Harmonic-generation processes are shown to be ideally suited for the non-linear spectroscopy and structure analysis of carbon nanotubes, in many ways supplementary to Raman spectroscopy. The second- and third-harmonic yields scale as quadratic and cubic functions, respectively, of the pump pulse energy up to pump intensities of 1012 W cm-2, indicating the perturbative regime of non-linear-optical interactions and suggesting a convenient calibration for the second and third harmonics employed as spectroscopic probes. Comparison of harmonic-generation data with absorption spectra of carbon-nanotube layers reveals an important role of quantum confinement effects in the non-linear coherent scattering of light from carbon nanotubes. Femtosecond pulses of Cr: forsterite laser radiation also generate the fifth optical harmonic at 251 nm in the glass substrate of carbon-nanotube samples, which can be employed for UV spectroscopy and subwavelength-resolution non-linear microscopy of carbon nanotubes. Copyright © 2003 John Wiley & Sons, Ltd.
Original languageEnglish
Pages (from-to)1018 - 1024
Number of pages7
JournalJournal of Raman Spectroscopy
Issue number12
Publication statusPublished - Dec 2003
Externally publishedYes


All Science Journal Classification (ASJC) codes

  • Spectroscopy

Cite this

Konorov, S. O., Akimov, D. A., Ivanov, A. A., Alfimov, M. V., Botti, S., Ciardi, R., ... Zheltikov, A. M. (2003). Femtosecond optical harmonic generation as a non-linear spectroscopic probe for carbon nanotubes. Journal of Raman Spectroscopy, 34(12), 1018 - 1024. https://doi.org/10.1002/jrs.1080