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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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| Item type | Article | ||||
| Journal or Publication Title | ACS Nano | ||||
| Publisher | AMER CHEMICAL SOC | ||||
| Open Access Type | Due to SHERPA/RoMEO | ||||
| Place of Publication | WASHINGTON | ||||
| Volume | 15 | ||||
| Number of Issue or Book Chapter | 11 | ||||
| Page Range | pp. 18037-18047 | ||||
| Date | 4 November 2021 | ||||
| Date of publication | 14 Dec 2021 10:47 | ||||
| Institutions | Physics > Institute of Experimental and Applied Physics > Chair Professor Lupton > Group John Lupton | ||||
| Identification Number |
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| Keywords | SINGLE-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 Classification | 500 Science > 530 Physics | ||||
| Status | Published | ||||
| Refereed | Yes, this version has been refereed | ||||
| Created at the University of Regensburg | Yes | ||||
| URN of the UB Regensburg | urn:nbn:de:bvb:355-epub-512071 | ||||
| Item ID | 51207 |
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