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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

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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Details

DokumentenartArtikel
Titel eines Journals oder einer ZeitschriftACS Nano
Verlag:AMER CHEMICAL SOC
Ort der Veröffentlichung:WASHINGTON
Band:15
Nummer des Zeitschriftenheftes oder des Kapitels:11
Seitenbereich:S. 18037-18047
Datum4 November 2021
InstitutionenPhysik > Institut für Experimentelle und Angewandte Physik > Lehrstuhl Professor Lupton > Arbeitsgruppe John Lupton
Identifikationsnummer
WertTyp
10.1021/acsnano.1c06649DOI
Stichwörter / 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-Dezimal-Klassifikation500 Naturwissenschaften und Mathematik > 530 Physik
StatusVeröffentlicht
BegutachtetJa, diese Version wurde begutachtet
An der Universität Regensburg entstandenJa
URN der UB Regensburgurn:nbn:de:bvb:355-epub-512071
Dokumenten-ID51207

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