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Hofmann, Felix J. ; Bodnarchuk, Maryna ; Protesescu, Loredana ; Kovalenko, Maksym ; Lupton, John M. ; Vogelsang, Jan

Exciton gating and triplet deshelving in single dye molecules excited by perovskite nanocrystal FRET antennae

Hofmann, Felix J., Bodnarchuk, Maryna , Protesescu, Loredana , Kovalenko, Maksym, Lupton, John M. and Vogelsang, Jan (2019) Exciton gating and triplet deshelving in single dye molecules excited by perovskite nanocrystal FRET antennae. The journal of physical chemistry letters 10 (5), pp. 1055-1062.

Date of publication of this fulltext: 08 Oct 2020 08:17
Article
DOI to cite this document: 10.5283/epub.43864


Abstract

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 resonance energy transfer (FRET). Here, we demonstrate ...

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 resonance energy transfer (FRET). Here, we demonstrate that FAPbBr(3) perovskite nanocrystals, of cuboidal shape and approximately 10 nm in size, are capable of selectively exciting single cyanine 3 molecules at a concentration 100-fold higher than standard single-molecule concentrations. This FRET antenna mechanism increases the effective brightness of the single dye molecules 100-fold. 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 1.5-fold compared to emission collected directly from the nanocrystals because 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 reverse intersystem crossing (RISC), 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 3.



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Details

Item typeArticle
Journal or Publication TitleThe journal of physical chemistry letters
Publisher:AMER CHEMICAL SOC
Place of Publication:WASHINGTON
Volume:10
Number of Issue or Book Chapter:5
Page Range:pp. 1055-1062
Date21 February 2019
InstitutionsPhysics > Institute of Experimental and Applied Physics > Chair Professor Lupton > Group John Lupton
Physics > Institute of Experimental and Applied Physics > Chair Professor Lupton > Group John Lupton
Identification Number
ValueType
10.1021/acs.jpclett.9b00180DOI
KeywordsRESONANCE ENERGY-TRANSFER; PHOTON EMISSION; HOMO-FRET; FLUORESCENCE; PHOTOLUMINESCENCE; ENHANCEMENT; PATHWAYS; BRIGHT; STATE;
Dewey Decimal Classification500 Science > 530 Physics
StatusPublished
RefereedYes, this version has been refereed
Created at the University of RegensburgYes
URN of the UB Regensburgurn:nbn:de:bvb:355-epub-438643
Item ID43864

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