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Photoswitchable single-walled carbon nanotubes for super-resolution microscopy in the near-infrared

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Science Advances  27 Sep 2019:
Vol. 5, no. 9, eaax1166
DOI: 10.1126/sciadv.aax1166
  • Fig. 1 UV irradiation induces luminescence intermittency on CNTs functionalized with SP-MC.

    (A) Schema representing the excitation and emission fluorescence setup with UV illumination. (B) Wide-field NIR image of (10,2) CNTs spin-coated on polyvinylpyrrolidone (PVP) illuminated with a 730 nm circular polarized laser (~10 kW/cm2). (C) Luminescence time traces showing that UV irradiation induces emission intermittency and reduces the mean intensity. Imaging rate = 20 Hz. (D) Time evolution of the average of 79 CNTs before and during UV irradiation. i.u., intensity units.

  • Fig. 2 Simulation modeling of the excitonic photophysical processes generating the luminescence.

    (A) Schematic representation of the nanotube functionalized with SP-MC molecules. An exciton generated in the middle of the nanotube and its probability of recombining are shown. Only excitons that recombine before encountering a merocyanine molecule or the end of the nanotube emit a photon. (B) The SP-MC group corresponds to a two-state model with transition rates defined as aSP = 1/tSP and aMC = 1/tMC. Simulated time traces are presented for φ =aMC/aSP = 100 with varying tSP (C) and for tMC = 50 s with varying φ (D). Simulated measurement rate = 20 Hz. Nanotube length and diffusion lengths were L = 300 nm, ld = 180 nm, and NSM = 1 per nm. The exciton generation rate was 133 nm−1 s−1.

  • Fig. 3 Characterization of the luminescence temporal time traces.

    (A) Graph showing the influence of the ratio φ = aMC/aSP for tMC = 50 s and ld = 180 nm on the ratio of the average luminescence intensities before and during the UV irradiation. The gray shaded area corresponds to the error on the estimation of φ for L = 300 ± 50 nm. (B) Examples of temporal ACFs for the time traces presented in Fig. 2 (C and D) for φ = 100 with varying tSP and for tMC = 50 s with varying φ. (C) Graph summarizing the impact of varying φ and tSP on the temporal autocorrelation decay constant. For Fig. 3 (A to C), L = 300 nm, ld = 180 nm, and NSM = 1 per nm. (D) Graph summarizing the impact of varying φ and tSP on the temporal autocorrelation decay constant plotted versus tcind=(tSPtMC)/(tSP+tMC). The slope tc=slopetcind is also shown in the inset as a function of φ. Values correspond to mean ± SD.

  • Fig. 4 Estimation of the switching rate dynamics of the SP-MC molecules from the intensity time trace of individual CNTs.

    (A) Four normalized intensity histograms and the corresponding temporal ACFs (B) for the CNTs shown in Fig. 1. (C and D) The histograms of the intensity ratio φ and tc, respectively, obtained from individual carbon nanotube luminescence time traces. Knowing φ and tc, the values of tSP (E) and tMC (F) can be estimated. Values correspond to mean ± SEM.

  • Fig. 5 Super-localization and super-resolution imaging of single CNTs using photocontrolled luminescence intermittency.

    Wide-field NIR zoomed images of (10,2) CNTs spin-coated on PVP illuminated with a 730 nm circular polarized laser (~10 kW/cm2). The zoomed regions of interests correspond to reconstructed super-localization of individual CNTs (A) and super-resolved image of closely located nanotubes (B) using intensity transitions from all the blinking steps in the acquired movies (20 Hz). The super-resolved image shows different nanotube segments ~320 nm apart that could not be resolved in the wide-field image. For display, each localization is convolved with a Gaussian having a ωFWHM = 50 nm.

Supplementary Materials

  • Supplementary material for this article is available at http://advances.sciencemag.org/cgi/content/full/5/9/eaax1166/DC1

    Movie S1. Movie showing the photoluminescence of single CNTs.

    Fig. S1. SP-MC nanotube hybrid.

    Fig. S2. SP-CNT luminescence in solution.

    Fig. S3. Theoretical modeling of the luminescence intensity of a nanotube with quencher molecules.

    Fig. S4. Influence of the residence times on the intensity ratio.

    Fig. S5. Error estimation of the parameter theoretical φ.

  • Supplementary Materials

    The PDF file includes:

    • Legend for movie S1
    • Fig. S1. SP-MC nanotube hybrid.
    • Fig. S2. SP-CNT luminescence in solution.
    • Fig. S3. Theoretical modeling of the luminescence intensity of a nanotube with quencher molecules.
    • Fig. S4. Influence of the residence times on the intensity ratio.
    • Fig. S5. Error estimation of the parameter theoretical φ.

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    Other Supplementary Material for this manuscript includes the following:

    • Movie S1 (.avi format). Movie showing the photoluminescence of single CNTs.

    Files in this Data Supplement:

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