Minimizing the luminescence lifetime while maintaining a high emission quantum yield is paramount in optimizing the excitation cross-section, radiative decay rate, and brightness of quantum solid-state light sources, particularly at room temperature, where non-radiative processes can dominate. In that sense, plasmon-based optical nanoantennas can feature strongly enhanced and confined optical fields to enhance excitation probabilities and fluorescence decay rates. Their morphology and their coupling to luminescent emitters can be engineered to minimize non-radiative losses and optimize their overall brightness.
We demonstrate here that short DNA strands are an excellent template to introduce individual fluorescent molecules in dimers of gold nanoparticles in order to achieve single photon emission with decay rates enhanced by more than two orders of magnitude (M. P. Busson et al, Nat. Commun. 3, 962 (2012)). The coupling between single dye molecules and plasmonic gap antennas can be further optimized by selecting nanostructures where the transition dipole of the emitter is aligned with the gold particle dimer axis (M. P. Busson & S. Bidault, Nano Lett. 14, 284 (2014)). Furthermore, by using dimers of 60 and 80 nm diameter gold particles, we demonstrate the assembly of nanostructures exhibiting single-photon emission with lifetimes that can fall below 10 ps and typical quantum yields in a 45−70% range (S. Bidault et al, ACS Nano 10, 4806 (2016)). These data are in excellent agreement with theoretical calculations and demonstrate that millions of bright fluorescent nanostructures, with radiative lifetimes below 100 ps, can be produced in parallel.
Sébastien Bidault, Alexis Devilez, Nicolas Bonod, and Jérôme Wenger, "Bright single-photon-emitting colloidal plasmonic nanostructures with picosecond lifetimes (Conference Presentation)," Proc. SPIE 10530, Ultrafast Phenomena and Nanophotonics XXII, 105300H (Presented at SPIE OPTO: January 30, 2018; Published: 14 March 2018); https://doi.org/10.1117/12.2286493.5751504654001.
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