Brightening of excitons in carbon nanotubes on dimensionality modification

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Abstract

Despite the attractive one-dimensional characteristics of carbon nanotubes1, their typically low luminescence quantum yield, restricted because of their one-dimensional nature2,3,4,5,6,7,8,9, has limited the performance of nanotube-based light-emitting devices10,11. Here, we report the striking brightening of excitons (bound electron–hole pairs)12,13 in carbon nanotubes through an artificial modification of their effective dimensionality from one dimension to zero dimensions. Exciton dynamics in carbon nanotubes with luminescent, local zero-dimension-like states generated by oxygen doping14 were studied as model systems. We found that the luminescence quantum yield of the excitons confined in the zero-dimension-like states can be more than at least one order larger (18%) than that of the intrinsic one-dimensional excitons (typically 1%), not only because of the reduced non-radiative decay pathways but also due to an enhanced radiative recombination probability beyond that of intrinsic one-dimensional excitons. Our findings are extendable to the realization of future nanoscale photonic devices including a near-infrared single-photon emitter operable at room temperature.

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Figure 1: Schematic of a carbon nanotube with a luminescent local state.
Figure 2: Optical spectra of carbon nanotubes with luminescent local states.
Figure 3: Relationship of luminescence intensities from mobile and local excitons.
Figure 4: Time-resolved and temperature-dependent luminescence studies.

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Acknowledgements

This research was supported by Precursory Research for Embryonic Science and Technology (PRESTO) programme (no. 3538 from the Japan Science and Technology Agency (JST)), by Grants-in-Aid for Scientific Research (nos 24681031, 22740195 and 23340085 from the Japan Society for the Promotion of Science (JSPS); no. 22016007 from the Ministry of Education, Culture, Sports, Science and Technology, Japan (MEXT)), and by Asahi Glass Foundation. The authors thank Y. Kawazoe, M. Uesugi, N. Tokitoh, T. Murakami, T. Umeyama and H. Imahori for experimental equipment and T. F. Heinz for discussions.

Author information

Y.M. developed the concept, designed the experiment and prepared the manuscript. Y.M. and M.I. performed the optical measurements. T.K. and M.O. contributed to the time-resolved photoluminescence measurements. M.I. prepared the samples. Y.M., M.I., S.M. and K.M. contributed to interpreting the results and writing the manuscript. All authors discussed the results and commented on the manuscript.

Correspondence to Yuhei Miyauchi.

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Miyauchi, Y., Iwamura, M., Mouri, S. et al. Brightening of excitons in carbon nanotubes on dimensionality modification. Nature Photon 7, 715–719 (2013) doi:10.1038/nphoton.2013.179

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