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Exciton antennas and concentrators from core–shell and corrugated carbon nanotube filaments of homogeneous composition

Nature Materials volume 9, pages 833–839 (2010)Cite this article

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Abstract

There has been renewed interest in solar concentrators and optical antennas for improvements in photovoltaic energy harvesting and new optoelectronic devices. In this work, we dielectrophoretically assemble single-walled carbon nanotubes (SWNTs) of homogeneous composition into aligned filaments that can exchange excitation energy, concentrating it to the centre of core–shell structures with radial gradients in the optical bandgap. We find an unusually sharp, reversible decay in photoemission that occurs as such filaments are cycled from ambient temperature to only 357 K, attributed to the strongly temperature-dependent second-order Auger process. Core–shell structures consisting of annular shells of mostly (6,5) SWNTs (Eg=1.21 eV) and cores with bandgaps smaller than those of the shell (Eg=1.17 eV (7,5)–0.98 eV (8,7)) demonstrate the concentration concept: broadband absorption in the ultraviolet–near-infrared wavelength regime provides quasi-singular photoemission at the (8,7) SWNTs. This approach demonstrates the potential of specifically designed collections of nanotubes to manipulate and concentrate excitons in unique ways.

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Figure 1: Optical properties of a (6,5)-enriched SWNT fibre: photoluminescence and strong EET.
Figure 2: PLE map and reversible photoluminescence change as a function of temperature.
Figure 3: Spatially resolved, temperature-dependent photoluminescence behaviour under an in-house-built dual-channel microscope.
Figure 4: Development of an exciton antenna from a core–shell carbon nanotube structure.

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Acknowledgements

M.S.S. is grateful for the NSF Career Award and the Sloan Fellowship for supporting this work. A grant to M.S.S. from the Dupont-MIT Alliance is appreciated. J-H.H. acknowledges support from the Korea Research Foundation (MOEHRD, KRF-2006-214-D00117). W-J.K. appreciates support from Kyungwon University. J.H.C. expresses his gratitude to Purdue University for financial support. The authors thank M. Zheng for useful discussions.

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Author notes

  1. Jae-Hee Han and Geraldine L. C. Paulus: These authors contributed equally to this work

Authors and Affiliations

  1. Department of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA

    Jae-Hee Han, Geraldine L. C. Paulus, Daniel A. Heller, Paul W. Barone, Chang Young Lee, Moon-Ho Ham, Changsik Song & Michael S. Strano

  2. Institute for Soldier Nanotechnologies, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA

    Jae-Hee Han, Chang Young Lee & Michael S. Strano

  3. Advanced Material Laboratories, Sony Corporation, Kanagawa, 243-0021, Japan

    Ryuichiro Maruyama

  4. Department of Energy and Biological Engineering, Kyungwon University, Seongnam, Gyeonggi-do 461-701, South Korea

    Woo-Jae Kim

  5. School of Mechanical Engineering, Birck Nanotechnology Center, Bindley Bioscience Center, Purdue University, West Lafayette, Indiana 47907, USA

    Jong Hyun Choi

  6. Departamento de Fı´sica, Universidade Federal de Minas Gerais, Belo Horizonte, MG 30123-970, Brazil

    C. Fantini

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  1. Jae-Hee Han
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Contributions

M.S.S. and J-H.H. conceived and designed the experiments. J-H.H. and G.L.C.P. carried out the experiments and theoretical calculation, and J-H.H., G.L.C.P. and M.S.S. analysed the data. D.A.H. designed and built the in-house dual-channel microscope. R.M., D.A.H., W-J.K., P.W.B., C.Y.L., J.H.C., M-H.H., C.S. and C.F. partly assisted in doing experiments and commented on the results. J-H.H., G.L.C.P. and M.S.S. wrote the paper.

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Correspondence to Michael S. Strano.

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The authors declare no competing financial interests.

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Han, JH., Paulus, G., Maruyama, R. et al. Exciton antennas and concentrators from core–shell and corrugated carbon nanotube filaments of homogeneous composition. Nature Mater 9, 833–839 (2010). https://doi.org/10.1038/nmat2832

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