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How Blinking Affects Photon Correlations in Multichromophoric Nanoparticles
Schröder, Tim, Bange, Sebastian
, Schedlbauer, Jakob, Steiner, Florian, Lupton, John M., Tinnefeld, Philip und Vogelsang, Jan
(2021)
How Blinking Affects Photon Correlations in Multichromophoric Nanoparticles.
ACS Nano 15 (11), S. 18037-18047.
Veröffentlichungsdatum dieses Volltextes: 14 Dez 2021 10:47
Artikel
DOI zum Zitieren dieses Dokuments: 10.5283/epub.51207
Zusammenfassung
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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| Dokumentenart | Artikel | ||||
| Titel eines Journals oder einer Zeitschrift | ACS Nano | ||||
| Verlag: | AMER CHEMICAL SOC | ||||
|---|---|---|---|---|---|
| Ort der Veröffentlichung: | WASHINGTON | ||||
| Band: | 15 | ||||
| Nummer des Zeitschriftenheftes oder des Kapitels: | 11 | ||||
| Seitenbereich: | S. 18037-18047 | ||||
| Datum | 4 November 2021 | ||||
| Institutionen | Physik > Institut für Experimentelle und Angewandte Physik > Lehrstuhl Professor Lupton > Arbeitsgruppe John Lupton | ||||
| Identifikationsnummer |
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| Stichwörter / 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-Dezimal-Klassifikation | 500 Naturwissenschaften und Mathematik > 530 Physik | ||||
| Status | Veröffentlicht | ||||
| Begutachtet | Ja, diese Version wurde begutachtet | ||||
| An der Universität Regensburg entstanden | Ja | ||||
| URN der UB Regensburg | urn:nbn:de:bvb:355-epub-512071 | ||||
| Dokumenten-ID | 51207 |
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