Abstract
Knowledge of excited-state dynamics in carbon nanotubes is determinant for their prospective use in optoelectronic applications. It is known that primary photoexcitations are quasi-one-dimensional excitons, the electron–hole correlation length (‘exciton size’) of which corresponds to a finite volume in the phase space. This volume can be directly measured by nonlinear spectroscopy provided the time resolution is short enough for probing before population relaxation. Here, we report on the experimental determination of exciton size and mobility in (6, 5) carbon nanotubes. The samples are sodium cholate suspensions of nanotubes (produced by the CoMoCat method) obtained by density-gradient ultracentrifugation. By using sub-15 fs near-infrared pulses to measure the nascent bleach of the lowest exciton resonance, we estimate the exciton size to be 2.0±0.7 nm. Exciton–exciton annihilation in our samples is found to be rather inefficient so that many excitons can coexist on a single nanotube.
This is a preview of subscription content, access via your institution
Access options
Subscribe to this journal
Receive 12 print issues and online access
$209.00 per year
only $17.42 per issue
Buy this article
- Purchase on Springer Link
- Instant access to full article PDF
Prices may be subject to local taxes which are calculated during checkout
Similar content being viewed by others
References
Wang, F., Dukovic, G., Brus, L. E. & Heinz, T. F. The optical resonances in carbon nanotubes arise from excitons. Science 308, 838–841 (2005).
Ando, T. Excitons in carbon nanotubes. J. Phys. Soc. Jpn 66, 1066–1073 (1997).
Perebeinos, V., Tersoff, J. & Avouris, P. Scaling of excitons in carbon nanotubes. Phys. Rev. Lett. 92, 257402 (2004).
Tretiak, S. et al. Excitons and Peierls distortion in conjugated carbon nanotubes. Nano Lett. 7, 86–92 (2007).
Chang, E., Bussi, G., Ruini, A. & Molinari, E. Excitons in carbon nanotubes: An ab initio symmetry-based approach. Phys. Rev. Lett. 92, 196401 (2004).
Korovyanko, O. J., Sheng, C.-X., Vardeny, Z.V., Dalton, A. B. & Baughman, R. H. Ultrafast spectroscopy of excitons in single-walled carbon nanotubes. Phys. Rev. Lett. 92, 017403 (2004).
Cognet, L. et al. Stepwise quenching of exciton fluorescence in carbon nanotubes by single-molecule reactions. Science 316, 1465–1468 (2007).
Wang, F., Dukovic, G., Knoesel, E., Brus, L. E. & Heinz, T. F. Observation of rapid Auger recombination in optically excited semiconducting carbon nanotubes. Phys. Rev. B 70, 241403(R) (2004).
Ma, Y.-Z., Valkunas, 1 L., Dexheimer, S. L., Bachilo, S. M. & Fleming, G. R. Femtosecond spectroscopy of optical excitations in single-walled carbon nanotubes: Evidence for exciton–exciton annihilation. Phys. Rev. Lett. 94, 157402 (2005).
Goesele, U. M. Reaction kinetics and diffusion in condensed matter. Prog. React. Kinetics 13, 63–161 (1984).
Greene, B. I., Orenstein, J. & Schmitt-Rink, S. All-optical nonlinearities in organics. Science 247, 679–687 (1990).
Zhu, Z. et al. Pump-probe spectroscopy of exciton dynamics in (6, 5) carbon nanotubes. J. Phys. Chem. C 111, 3831–2825 (2007).
Schmitt-Rink, S., Chemla, D. S. & Miller, D. A. B. Theory of transient excitonic optical nonlinearities in semiconductor quantum-well structures. Phys. Rev. B 32, 6601–6609 (1985).
Capaz, R. B., Spataru, C. D., Beigi, S. I. & Louie, S. G. Diameter and chirality dependence of exciton properties in carbon nanotubes. Phys. Rev. B 74, 121401, R (2006).
Zheng, M. & Diner, A. Solution redox chemistry of carbon nanotubes. J. Am. Chem. Soc. 126, 15490–15494 (2004).
Manzoni, C. et al. Intersubband exciton relaxation dynamics in single-walled carbon nanotubes. Phys. Rev. Lett. 94, 207401 (2005).
Hagen, A. et al. Phys. Rev. Lett. 95, 197401 (2005).
Crochet, J., Clemens, M. & Hertel, T. Quantum yield heterogeneities of aqueous single-wall carbon nanotube suspensions. J. Am. Chem. Soc. 129, 8058–8059 (2007).
Manzoni, C., Polli, D. & Cerullo, G. Two-color pump-probe system broadly tunable over the visible and the near infrared with sub-30 fs temporal resolution. Rev. Sci. Instrum. 77, 023103 (2006).
Polli, D., Lüer, L. & Cerullo, G. High-time-resolution pump-probe system with broadband detection for the study of time-domain vibrational dynamics. Rev. Sci. Instrum. 78, 103108 (2007).
Acknowledgements
This work was financially supported by the European Commission through the Human Potential Programme (Marie-Curie RTN BIMORE, Grant No. MRTN-CT-2006-035859) and by the National Science Foundation (NSF DMR-0606505). We acknowledge the financial support of the project FIRB SYNERGY.
Author information
Authors and Affiliations
Contributions
All authors contributed significantly to this work. In detail, project planning by G.L. and T.H., sample preparation and characterization by J.C. and T.H., measurement set-up and automation by D.P. and L.L., experiments by L.L. and S.H., data evaluation by L.L., G.L. and S.H., manuscript writing by L.L., G.L., T.H. and D.P.
Corresponding author
Supplementary information
Supplementary Information
Supplementary Informations (PDF 249 kb)
Rights and permissions
About this article
Cite this article
Lüer, L., Hoseinkhani, S., Polli, D. et al. Size and mobility of excitons in (6, 5) carbon nanotubes. Nature Phys 5, 54–58 (2009). https://doi.org/10.1038/nphys1149
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1038/nphys1149
This article is cited by
-
Resonant exciton transfer in mixed-dimensional heterostructures for overcoming dimensional restrictions in optical processes
Nature Communications (2023)
-
Conversion of twisted light to twisted excitons using carbon nanotubes
npj Computational Materials (2022)
-
Bandgap renormalization in single-wall carbon nanotubes
Scientific Reports (2017)
-
Enhancement of Photoluminescence from Semiconducting Nanotubes in Aqueous Suspensions due to Cysteine and Dithiothreitol Doping: Influence of the Sonication Treatment
Nanoscale Research Letters (2016)
-
Exciton–exciton annihilation and biexciton stimulated emission in graphene nanoribbons
Nature Communications (2016)