SCIENCE@home

Ultrafast single-molecule fluorescence measured by femtosecond double-pulse excitation photon antibunching.

Jakob Schedlbauer,P. Wilhelm,Lennart Grabenhorst,Marie-Elisabeth Federl,B. Lalkens,Florian Hinderer,Ullrich Scherf,Sigurd Höger,P. Tinnefeld,S. Bange,J. Vogelsang,J. Lupton

Published 2019 in Nano letters (Print)

ABSTRACT

Most measurements of fluorescence lifetimes on the single-molecule level are carried out using avalanche photon diodes (APDs). These single-photon counters are inherently slow and their response shows a strong dependence on photon energy, which can make deconvolution of the instrument response function (IRF) challenging. An ultrafast time resolution in single-molecule fluorescence is crucial, e.g., in determining donor lifetimes in donor-acceptor couples which undergo energy transfer, or in plasmonic antenna structures, where the radiative rate is enhanced. We introduce a femtosecond double-excitation (FeDEx) photon correlation technique, which measures the degree of photon antibunching as a function of time delay between two excitation pulses. In this boxcar integration, the time resolution of fluorescence transients is limited solely by the laser pulse length and is independent of the detector IRF. The versatility of the technique is demonstrated with a custom-made donor acceptor complex with one donor and two acceptors; and with single dye molecules positioned accurately between two gold nanoparticles using DNA origami. The latter structures show ~75-fold radiative-rate enhancements and fluorescence lifetimes of down to 17 ps, which is measured without the need of any deconvolution. With the potential of measuring sub-picosecond fluorescence lifetimes plasmonic antenna structures can now be optimized further.

PUBLICATION RECORD

CITATION MAP

EXTRACTION MAP

CLAIMS

  • No claims are published for this paper.

CONCEPTS

  • No concepts are published for this paper.

REFERENCES

Showing 1-36 of 36 references · Page 1 of 1

CITED BY

Showing 1-24 of 24 citing papers · Page 1 of 1