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Schröder, Tim ; Bange, Sebastian ; Schedlbauer, Jakob ; Steiner, Florian ; Lupton, John M. ; Tinnefeld, Philip ; Vogelsang, Jan

How Blinking Affects Photon Correlations in Multichromophoric Nanoparticles

Article

Schröder, Tim, Bange, Sebastian , Schedlbauer, Jakob, Steiner, Florian, Lupton, John M., Tinnefeld, Philip and Vogelsang, Jan (2021) How Blinking Affects Photon Correlations in Multichromophoric Nanoparticles. ACS Nano 15 (11), pp. 18037-18047.

DOI to cite this document: 10.5283/epub.51207


Abstract

A single chromophore can only emit a maximum of one single photon per excitation cycle. This limitation results in a phenomenon commonly referred to as photon antibunching (pAB). When multiple chromophores contribute to the fluorescence measured, the degree of pAB has been used as a metric to "count" the number of chromophores. But the fact that chromophores can switch randomly between bright and ...

A single chromophore can only emit a maximum of one single photon per excitation cycle. This limitation results in a phenomenon commonly referred to as photon antibunching (pAB). When multiple chromophores contribute to the fluorescence measured, the degree of pAB has been used as a metric to "count" the number of chromophores. But the fact that chromophores can switch randomly between bright and dark states also impacts pAB and can lead to incorrect chromophore numbers being determined from pAB measurements. By both simulations and experiment, we demonstrate how pAB is affected by independent and collective chromophore blinking, enabling us to formulate universal guidelines for correct interpretation of pAB measurements. We use DNA-origami nanostructures to design multichromophoric model systems that exhibit either independent or collective chromophore blinking. Two approaches are presented that can distinguish experimentally between these two blinking mechanisms. The first one utilizes the different excitation intensity dependence on the blinking mechanisms. The second approach exploits the fact that collective blinking implies energy transfer to a quenching moiety, which is a time-dependent process. In pulsed-excitation experiments, the degree of collective blinking can therefore be altered by time gating the fluorescence photon stream, enabling us to extract the energy-transfer rate to a quencher. The ability to distinguish between different blinking mechanisms is valuable in materials science, such as for multichromophoric nanoparticles like conjugated-polymer chains as well as in biophysics, for example, for quantitative analysis of protein assemblies by counting chromophores.



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Details

Item typeArticle
Journal or Publication TitleACS Nano
PublisherAMER CHEMICAL SOC
Open Access TypeDue to SHERPA/RoMEO
Place of PublicationWASHINGTON
Volume15
Number of Issue or Book Chapter11
Page Rangepp. 18037-18047
Date4 November 2021
Date of publication14 Dec 2021 10:47
InstitutionsPhysics > Institute of Experimental and Applied Physics > Chair Professor Lupton > Group John Lupton
Identification Number
ValueType
10.1021/acsnano.1c06649DOI
KeywordsSINGLE-MOLECULE FLUORESCENCE; ENERGY-TRANSFER; SPECTROSCOPY; STATISTICS; MECHANISM; EMITTERS; POLYMER; PHOTOPHYSICS; PATHWAYS; TRIPLET; single-molecule spectroscopy; photon statistics; DNA-origami structures; photophysics; quantum optics
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-512071
Item ID51207

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