期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 116, 期 10, 页码 4064-4069出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1808290116
关键词
single molecule; fluorescence; spectroscopy; energy transfer; correlations
资金
- Danish Council of Independent Research [DFF-7014-00027]
- Austrian Science Fund (FWF): START project [Y631-N27]
- Laserlab-Europe [EUH2020 654148]
- European Research Council [291198, 648615, 754802]
- European Research Council (ERC) [648615, 754802] Funding Source: European Research Council (ERC)
- Austrian Science Fund (FWF) [Y631] Funding Source: Austrian Science Fund (FWF)
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.
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