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Giant Raman scattering from J-aggregated dyes inside carbon nanotubes for multispectral imaging


Raman spectroscopy uses visible light to acquire vibrational fingerprints of molecules, thus making it a powerful tool for chemical analysis in a wide range of media. However, its potential for optical imaging at high resolution is severely limited by the fact that the Raman effect is weak. Here, we report the discovery of a giant Raman scattering effect from encapsulated and aggregated dye molecules inside single-walled carbon nanotubes. Measurements performed on rod-like dyes such as α-sexithiophene and β-carotene, assembled inside single-walled carbon nanotubes as highly polarizable J-aggregates, indicate a resonant Raman cross-section of (3 ± 2) × 10−21 cm2 sr−1, which is well above the cross-section required for detecting individual aggregates at the highest optical resolution. Free from fluorescence background and photobleaching, this giant Raman effect allows the realization of a library of functionalized nanoprobe labels for Raman imaging with robust detection using multispectral analysis.

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Figure 1: Schematic representation of 6T@f-SWNT.
Figure 2: Absorbance and Raman spectra of SWNTs, 6T, 6T@SWNTs and 6T@f-SWNTs.
Figure 3: Polarized micro-Raman spectroscopy of individual SWNTs.
Figure 4: Demonstration of dyes@SWNTs as Raman nanoprobes.
Figure 5: Raman multiplexing, protein recognition and tagged bacteria with dyes@SWNTs nanoprobes.


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The authors thank M. Côté, P. McBreen and C. Silva for discussions, M. Choueb for SEM, B. Simard and his group for providing the SWNTs used for this study, M.A. Loi and E. Menna for sharing samples of 6T@SWNTs and discussions, and J. Barbeau for providing cultures of Candida albicans. This work was possible because of financial support from the Natural Sciences and Engineering Research Council of Canada (NSERC), Nanoquébec and the Canada Research Chair (CRC) programmes.

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Data were collected and analysed by E.G., N.Y.-Wa.T., F.L., J.C., M.-A.N. and R.M. The experiments were conceived by E.G., N.Y.-Wa.T., J.C., F.L., M.-A.N. and R.M. Calculations were carried out by E.G., T.S. and R.M. Samples were prepared by N.Y.-Wa.T., E.G., N.C., F.L., F.R., J.C. and M.-A.N. All authors contributed to writing the manuscript.

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Correspondence to R. Martel.

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The authors declare no competing financial interests.

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Gaufrès, E., Tang, NW., Lapointe, F. et al. Giant Raman scattering from J-aggregated dyes inside carbon nanotubes for multispectral imaging. Nature Photon 8, 72–78 (2014).

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