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Single-molecule excitation–emission spectroscopy

Thyrhaug, Erling ; Krause, Stefan ; Perri, Antonio ; Cerullo, Giulio ; Polli, Dario ; Vosch, Tom ; Hauer, Jürgen

Proceedings of the National Academy of Sciences - PNAS, 2019-03, Vol.116 (10), p.4064-4069 [Periódico revisado por pares]

United States: National Academy of Sciences

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  • Título:
    Single-molecule excitation–emission spectroscopy
  • Autor: Thyrhaug, Erling ; Krause, Stefan ; Perri, Antonio ; Cerullo, Giulio ; Polli, Dario ; Vosch, Tom ; Hauer, Jürgen
  • Assuntos: Broadband ; Diimide ; Emission spectra ; Emission spectroscopy ; Emitters ; Excitation spectra ; Fluorescence ; Physical Sciences ; Polystyrene ; Polystyrene resins ; Recording ; Spectral emittance ; Spectroscopy ; Spectrum analysis ; Variation
  • É parte de: Proceedings of the National Academy of Sciences - PNAS, 2019-03, Vol.116 (10), p.4064-4069
  • Notas: ObjectType-Article-1
    SourceType-Scholarly Journals-1
    ObjectType-Feature-2
    content type line 23
    Author contributions: E.T., G.C., D.P., T.V., and J.H. designed research; E.T., S.K., and A.P. performed research; E.T., S.K., and A.P. analyzed data; and E.T. wrote the paper.
    Edited by Shaul Mukamel, University of California, Irvine, CA, and approved January 17, 2019 (received for review May 14, 2018)
  • Descrição: Single-molecule spectroscopy (SMS) provides a detailed view of individual emitter properties and local environments without having to resort to ensemble averaging. While the last several decades have seen substantial refinement of SMS techniques, recording excitation spectra of single emitters still poses a significant challenge. Here we address this problem by demonstrating simultaneous collection of fluorescence emission and excitation spectra using a compact common-path interferometer and broadband excitation, which is implemented as an extension of a standard SMS microscope. We demonstrate the technique by simultaneously collecting room-temperature excitation and emission spectra of individual terrylene diimide molecules and donor– acceptor dyads embedded in polystyrene. We analyze the resulting spectral parameters in terms of optical lineshape theory to obtain detailed information on the interactions of the emitters with their nanoscopic environment. This analysis finally reveals that environmental fluctuations between the donor and acceptor in the dyads are not correlated.
  • Editor: United States: National Academy of Sciences
  • Idioma: Inglês
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