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Single-molecule excitation-emission spectroscopy.


ABSTRACT: 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.

SUBMITTER: Thyrhaug E 

PROVIDER: S-EPMC6410781 | biostudies-literature | 2019 Mar

REPOSITORIES: biostudies-literature

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Single-molecule excitation-emission spectroscopy.

Thyrhaug Erling E   Krause Stefan S   Perri Antonio A   Cerullo Giulio G   Polli Dario D   Vosch Tom T   Hauer Jürgen J  

Proceedings of the National Academy of Sciences of the United States of America 20190215 10


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 bro  ...[more]

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