Spectral dynamics and spatial localization of single molecules in a polymer

We report on the high-resolution spectroscopy of single dibenzanthanthrene molecules embedded in polymethyl methacrylate (PMMA). We employed three methods for the characterization of spectral line shapes based on fitting a Lorentzian function, determining full widths at half-maxima, and calculation of the second-order spectral cumulant. The three approaches provide comparable histograms of linewidth distributions, displaying slowly decaying tails that are indicative of the Lévy stable law. In addition, we introduce an alternative method for the analysis of spectral dynamics, in which ensemble spectra are reconstructed by adding single molecule spectral autocorrelations. Furthermore, we examine the spectral width and distributions of single molecules on the PMMA chain length over three orders of magnitude and find a very small dependence. Lastly, we demonstrate that, despite the strong spectral dynamics, it is possible to collect enough photons from single molecules to localize their positions to better than 10 nm.

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