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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 (_E_g=1.21
eV) and cores with bandgaps smaller than those of the shell (_E_g=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. Access through your institution Buy or subscribe This is a preview of subscription content, access via your institution ACCESS OPTIONS Access through
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Read our FAQs * Contact customer support SIMILAR CONTENT BEING VIEWED BY OTHERS THERMAL AND NONTHERMAL EXCITON LIGHT EMISSIONS FROM CARBON NANOTUBES ABOVE 1000 K Article Open access 01 May
2025 RESONANT EXCITON TRANSFER IN MIXED-DIMENSIONAL HETEROSTRUCTURES FOR OVERCOMING DIMENSIONAL RESTRICTIONS IN OPTICAL PROCESSES Article Open access 09 December 2023 GIANT BULK PHOTOVOLTAIC
EFFECT DRIVEN BY THE WALL-TO-WALL CHARGE SHIFT IN WS2 NANOTUBES Article Open access 10 June 2022 REFERENCES * Currie, M. J., Mapel, J. K., Heidel, T. D., Goffri, S. & Baldo, M. A.
High-efficiency organic solar concentrators for photovoltaics. _Science_ 321, 226–228 (2008). Article CAS Google Scholar * Yoon, J. et al. Ultrathin silicon solar microcells for
semitransparent, mechanically flexible and microconcentrator module designs. _Nature Mater._ 7, 907–915 (2008). Article CAS Google Scholar * Mühlschlegel, P., Eisler, H-J., Martin, O. J.
F., Hecht, B. & Pohl, D. W. Resonant optical antennas. _Science_ 308, 1607–1609 (2005). Article Google Scholar * Taminiau, T. H., Stefani, F. D., Segerink, F. B. & van Hulst, N. F.
Optical antennas direct single-molecule emission. _Nature Photon._ 2, 234–237 (2008). Article CAS Google Scholar * van de Lagemaat, J. et al. Organic solar cells with carbon nanotubes
replacing In2O3:Sn as the transparent electrode. _Appl. Phys. Lett._ 88, 233503 (2006). Article Google Scholar * Schuller, J. A., Taubner, T. & Brongersma, M. L. Optical antenna
thermal emitters. _Nature Photon._ 3, 658–661 (2009). Article CAS Google Scholar * Lin, M. F. Optical spectra of single-wall carbon nanotube bundles. _Phys. Rev. B_ 62, 13153–13159
(2000). Article CAS Google Scholar * Yu, Z. & Brus, L. Rayleigh and Raman scattering from individual carbon nanotube bundles. _J. Phys. Chem. B_ 105, 1123–1134 (2001). Article CAS
Google Scholar * Wang, F. et al. Interactions between individual carbon nanotubes studied by Rayleigh scattering spectroscopy. _Phys. Rev. Lett._ 96, 167401 (2006). Article Google Scholar
* Tan, P. H. et al. Photoluminescence spectroscopy of carbon nanotube bundles: Evidence for exciton energy transfer. _Phys. Rev. Lett._ 99, 137402 (2007). Article CAS Google Scholar *
Qian, H. et al. Exciton transfer and propagation in carbon nanotubes studied by near-field optical microscopy. _Phys. Status Solidi B_ 245, 2243–2246 (2008). Article CAS Google Scholar *
Kato, T. & Hatakeyama, R. Exciton energy transfer-assisted photoluminescence brightening from freestanding single-walled carbon nanotube bundles. _J. Am. Chem. Soc._ 130, 8101–8107
(2008). Article CAS Google Scholar * Lefebvre, J. & Finnie, P. Photoluminescence and Förster resonance energy transfer in elemental bundles of single-walled carbon nanotubes. _J.
Phys. Chem. C_ 113, 7536–7540 (2009). Article CAS Google Scholar * Delaney, P., Choi, H. J., Ihm, J., Louie, S. G. & Cohen, M. L. Broken symmetry and pseudogaps in ropes of carbon
nanotubes. _Phys. Rev. B_ 60, 7899–7904 (1999). Article CAS Google Scholar * Kim, W-J., Nair, N., Lee, C. Y. & Strano, M. S. Covalent functionalization of single-walled carbon
nanotubes alters their densities allowing electronic and other types of separation. _J. Phys. Chem. C_ 112, 7326–7331 (2008). Article CAS Google Scholar * Arnold, M. S., Green, A. A.,
Hulvat, J. F., Stupp, S. I. & Hersam, M. C. Sorting carbon nanotubes by electronic structure using density differentiation. _Nature Nanotech._ 1, 60–65 (2006). Article CAS Google
Scholar * Förster, T. 10th Spiers Memorial Lecture. Transfer mechanisms of electronic excitation. _Discuss. Faraday Soc._ 27, 7–17 (1959). Article Google Scholar * Scardaci, V. et al.
Carbon nanotubes for ultrafast photonics. _Phys. Status Solidi B_ 244, 4303–4307 (2007). Article CAS Google Scholar * Hertel, T., Fasel, R. & Moos, G. Charge-carrier dynamics in
single-wall carbon nanotube bundles: A time-domain study. _Appl. Phys. A_ 75, 449–465 (2002). Article CAS Google Scholar * Lauret, J-S. et al. Ultrafast carrier dynamics in single-wall
carbon nanotubes. _Phys. Rev. Lett._ 90, 057404 (2003). Article Google Scholar * Tang, J. et al. Assembly of 1D nanostructures into sub-micrometer diameter fibrils with controlled and
variable length by dielectrophoresis. _Adv. Mater._ 15, 1352–1355 (2003). Article CAS Google Scholar * Wang, F., Dukovic, G., Brus, L. E. & Heinz, T. F. Time-resolved fluorescence of
carbon nanotubes and its implication for radiative lifetimes. _Phys. Rev. Lett._ 92, 177401 (2004). Article Google Scholar * Perebeinos, V., Tersoff, J. & Avouris, P. Radiative
lifetime of excitons in carbon nanotubes. _Nano Lett._ 5, 2495–2499 (2005). Article CAS Google Scholar * Qian, H. et al. Exciton energy transfer in pairs of single-walled carbon
nanotubes. _Nano Lett._ 8, 1363–1367 (2008). Article CAS Google Scholar * Uchida, T., Tachibana, M. & Kojima, K. Thermal relaxation kinetics of defects in single-wall carbon
nanotubes. _J. Appl. Phys._ 101, 084313 (2007). Article Google Scholar * Hagen, A. et al. Exponential decay lifetimes of excitons in individual single-walled carbon nanotubes. _Phys. Rev.
Lett._ 95, 197401 (2005). Article Google Scholar * Trautz, M. Das Gesetz der Reaktionsgeschwindigkeit und der Gleichgewichte in Gasen. Bestätigung der Additivität von Cv-3/2R. Neue
Bestimmung der Integrationskonstanten und der Moleküldurchmesser. _Z. Anorg. Allg. Chem._ 96, 1–28 (1916). Article CAS Google Scholar * Manzoni, C. et al. Intersubband exciton relaxation
dynamics in single-walled carbon nanotubes. _Phys. Rev. Lett._ 94, 207401 (2005). Article CAS Google Scholar * Vyazovkin, S. Kinetic concepts of thermally stimulated reactions in solids:
A view from a historical perspective. _Int. Rev. Phys. Chem._ 19, 45–60 (2000). Article CAS Google Scholar * Jost, W. The theory of electrolytical charge and diffusion in crystals. II.
_Z. Phys. Chem. A_ 169, 129–134 (1934). Google Scholar * Zeldowitsch, J. B. On the theory of reactions on powders and porous substances. _Acta Phys.-Chim. URSS_ 10, 583–592 (1939). Google
Scholar * O’Connell, M. J. et al. Band gap fluorescence from individual single-walled carbon nanotubes. _Science_ 297, 593–596 (2002). Article Google Scholar * Buehler, M. J. Mesoscale
modeling of mechanics of carbon nanotubes: Self-assembly, self-folding, and fracture. _J. Mater. Res._ 21, 2855–2869 (2006). Article CAS Google Scholar * Kroeze, J. E., Koehorst, R. B. M.
& Savenije, T. J. Singlet and triplet exciton diffusion in a self-organizing porphyrin antenna layer. _Adv. Funct. Mater._ 14, 992–998 (2004). Article CAS Google Scholar * Gottfried,
D. S., Steffen, M. A. & Boxer, S. G. Large protein-induced dipoles for a symmetric carotenoid in a photosynthetic antenna complex. _Science_ 251, 662–665 (1991). Article CAS Google
Scholar * Abdula, D. & Shim, M. Performance and photovoltaic response of polymer-doped carbon nanotube p–n diodes. _ACS Nano_ 2, 2154–2159 (2008). Article CAS Google Scholar * Bibby,
T. S., Nield, J., Partensky, F. & Barber, J. Oxyphotobacteria: Antenna ring around photosystem I. _Nature_ 413, 590 (2001). Article CAS Google Scholar * Green, B. R. & Parson, W.
W. _Light-Harvesting Antennas in Photosynthesis_, VOL. 13 (Kluwer Academic, 2003). Book Google Scholar Download references 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. AUTHOR INFORMATION Author notes * Jae-Hee Han and Geraldine L. C. Paulus: These authors contributed equally to this work AUTHORS AND AFFILIATIONS * 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 * Institute for Soldier Nanotechnologies, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA Jae-Hee Han, Chang Young Lee &
Michael S. Strano * Advanced Material Laboratories, Sony Corporation, Kanagawa, 243-0021, Japan Ryuichiro Maruyama * Department of Energy and Biological Engineering, Kyungwon University,
Seongnam, Gyeonggi-do 461-701, South Korea Woo-Jae Kim * School of Mechanical Engineering, Birck Nanotechnology Center, Bindley Bioscience Center, Purdue University, West Lafayette, Indiana
47907, USA Jong Hyun Choi * Departamento de Fı´sica, Universidade Federal de Minas Gerais, Belo Horizonte, MG 30123-970, Brazil C. Fantini Authors * Jae-Hee Han View author publications You
can also search for this author inPubMed Google Scholar * Geraldine L. C. Paulus View author publications You can also search for this author inPubMed Google Scholar * Ryuichiro Maruyama
View author publications You can also search for this author inPubMed Google Scholar * Daniel A. Heller View author publications You can also search for this author inPubMed Google Scholar *
Woo-Jae Kim View author publications You can also search for this author inPubMed Google Scholar * Paul W. Barone View author publications You can also search for this author inPubMed
Google Scholar * Chang Young Lee View author publications You can also search for this author inPubMed Google Scholar * Jong Hyun Choi View author publications You can also search for this
author inPubMed Google Scholar * Moon-Ho Ham View author publications You can also search for this author inPubMed Google Scholar * Changsik Song View author publications You can also search
for this author inPubMed Google Scholar * C. Fantini View author publications You can also search for this author inPubMed Google Scholar * Michael S. Strano View author publications You
can also search for this author inPubMed Google Scholar 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. CORRESPONDING AUTHOR Correspondence to Michael S.
Strano. ETHICS DECLARATIONS COMPETING INTERESTS The authors declare no competing financial interests. SUPPLEMENTARY INFORMATION SUPPLEMENTARY INFORMATION Supplementary Information (PDF 966
kb) RIGHTS AND PERMISSIONS Reprints and permissions ABOUT THIS ARTICLE CITE THIS ARTICLE 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 Download citation * Received: 10 December 2009 * Accepted:
13 July 2010 * Published: 12 September 2010 * Issue Date: October 2010 * DOI: https://doi.org/10.1038/nmat2832 SHARE THIS ARTICLE Anyone you share the following link with will be able to
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