Exciton dynamics in semiconducting carbon nanotubes

M. W. Graham, J. Chmeliov, Y. Z. Ma, H. Shinohara, A. A. Green, Mark C Hersam, L. Valkunas, G. R. Fleming

Research output: Contribution to journalArticle

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Abstract

We report a femtosecond transient absorption spectroscopic study on the (6, 5) single-walled carbon nanotubes and the (7, 5) inner tubes of a dominant double-walled carbon nanotube species. We found that the dynamics of exciton relaxation probed at the ?rst transition-allowed state (E11) of a given tube type exhibits a markedly slower decay when the second transition-allowed state (E22) is excited than that measured by exciting its ?rst transition-allowed state (E11). A linear intensity dependence of the maximal amplitude of the transient absorption signal is found for the E22 excitation, whereas the corresponding amplitude scales linearly with the square root of the E11 excitation intensity. Theoretical modeling of these experimental ?ndings was performed by developing a continuum model and a stochastic model with explicit consideration of the annihilation of coherent excitons. Our detailed numerical simulations show that both models can reproduce reasonably well the initial portion of decay kinetics measured upon the E22 and E11 excitation of the chosen tube species, but the stochastic model gives qualitatively better agreement with the intensity dependence observed experimentally than those obtained with the continuum model.

Original languageEnglish
Pages (from-to)5201-5211
Number of pages11
JournalJournal of Physical Chemistry B
Volume115
Issue number18
DOIs
Publication statusPublished - May 12 2011

Fingerprint

Carbon Nanotubes
Excitons
Carbon nanotubes
carbon nanotubes
excitons
Stochastic models
tubes
Single-walled carbon nanotubes (SWCN)
Electron transitions
continuums
excitation
decay
Kinetics
Computer simulation
LDS 751
kinetics
simulation

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Materials Chemistry
  • Surfaces, Coatings and Films

Cite this

Graham, M. W., Chmeliov, J., Ma, Y. Z., Shinohara, H., Green, A. A., Hersam, M. C., ... Fleming, G. R. (2011). Exciton dynamics in semiconducting carbon nanotubes. Journal of Physical Chemistry B, 115(18), 5201-5211. https://doi.org/10.1021/jp106250a

Exciton dynamics in semiconducting carbon nanotubes. / Graham, M. W.; Chmeliov, J.; Ma, Y. Z.; Shinohara, H.; Green, A. A.; Hersam, Mark C; Valkunas, L.; Fleming, G. R.

In: Journal of Physical Chemistry B, Vol. 115, No. 18, 12.05.2011, p. 5201-5211.

Research output: Contribution to journalArticle

Graham, MW, Chmeliov, J, Ma, YZ, Shinohara, H, Green, AA, Hersam, MC, Valkunas, L & Fleming, GR 2011, 'Exciton dynamics in semiconducting carbon nanotubes', Journal of Physical Chemistry B, vol. 115, no. 18, pp. 5201-5211. https://doi.org/10.1021/jp106250a
Graham MW, Chmeliov J, Ma YZ, Shinohara H, Green AA, Hersam MC et al. Exciton dynamics in semiconducting carbon nanotubes. Journal of Physical Chemistry B. 2011 May 12;115(18):5201-5211. https://doi.org/10.1021/jp106250a
Graham, M. W. ; Chmeliov, J. ; Ma, Y. Z. ; Shinohara, H. ; Green, A. A. ; Hersam, Mark C ; Valkunas, L. ; Fleming, G. R. / Exciton dynamics in semiconducting carbon nanotubes. In: Journal of Physical Chemistry B. 2011 ; Vol. 115, No. 18. pp. 5201-5211.
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