Exciton Gating and Triplet Deshelving in Single Dye Molecules Excited by Perovskite Nanocrystal FRET Antennae

Felix J. Hofmann^a, Maryna I. Bodnarchuk^b^,^c, Loredana Protesescu^b^,^c, Maksym V. Kovalenko^b^,^c, John M. Lupton^a, Jan Vogelsang^d

^aInstitut für Experimentelle und Angewandte Physik, Universität Regensburg, Universitätsstraße 31, 93053 Regensburg, Germany

^bETH Zürich, Department of Chemistry and Applied Biosciences, Switzerland, Switzerland

^cEMPA - Swiss Federal Laboratories for Materials Science and Technology, Überland Strasse, 129, Dübendorf, Switzerland

^dLudwig-Maximilians-Universität München, Department Chemie, Germany, Butenandtstraße, 5-13, München, Germany

Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe Fall Meeting 2018 (NFM18)

S5 Charge Carrier Dynamics at the Nanoscale

Torremolinos, Spain, 2018 October 22nd - 26th

Organizers: David Egger, Arjan Houtepen and Freddy Rabouw

Oral, Felix J. Hofmann, presentation 246
DOI: https://doi.org/10.29363/nanoge.nfm.2018.246
Publication date: 6th July 2018

The extraordinary absorption cross-section and high photoluminescence (PL) quantum yield of perovskite nanocrystals make this type of material attractive to a variety of applications in optoelectronics. For the same reasons, nanocrystals are also ideally suited to function as nanoantennae to excite nearby single dye molecules by fluorescence resonant energy transfer (FRET). Here, we demonstrate that FAPbBr3 perovskite nanocrystals, of cuboidal shape and approximately 10 nm in size, are capable of selectively exciting single Cyanin 3 molecules at a concentration a hundredfold higher than standard single-molecule concentrations. This FRET antenna mechanism increases the effective brightness of the single dye molecules one hundredfold. Photon statistics and emission polarization measurements provide evidence for the FRET process by revealing photon-antibunching with unprecedented fidelity and highly polarized emission stemming from single dye molecules. Remarkably, the quality of single-photon emission improves two-fold compared to emission collected directly from the nanocrystals since the higher excited states of the dye molecule act as effective filters to multiexcitons. The same process gives rise to efficient deshelving of the molecular triplet state by reversed intersystem crossing, translating into a reduction of the PL saturation of the dye, thereby increasing the maximum achievable PL intensity of the dye by a factor of five.

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