Direkt zum Inhalt

Hedley, Gordon J. ; Schröder, Tim ; Steiner, Florian ; Eder, Theresa ; Hofmann, Felix J. ; Bange, Sebastian ; Laux, Dirk ; Höger, Sigurd ; Tinnefeld, Philip ; Lupton, John M. ; Vogelsang, Jan

Picosecond time-resolved photon antibunching measures nanoscale exciton motion and the true number of chromophores

Hedley, Gordon J., Schröder, Tim, Steiner, Florian, Eder, Theresa, Hofmann, Felix J., Bange, Sebastian, Laux, Dirk, Höger, Sigurd, Tinnefeld, Philip, Lupton, John M. und Vogelsang, Jan (2021) Picosecond time-resolved photon antibunching measures nanoscale exciton motion and the true number of chromophores. Nature Communications 12 (1), S. 1-10.

Veröffentlichungsdatum dieses Volltextes: 15 Jul 2021 16:42
Artikel
DOI zum Zitieren dieses Dokuments: 10.5283/epub.46377


Zusammenfassung

The particle-like nature of light becomes evident in the photon statistics of fluorescence from single quantum systems as photon antibunching. In multichromophoric systems, exciton diffusion and subsequent annihilation occurs. These processes also yield photon antibunching but cannot be interpreted reliably. Here we develop picosecond time-resolved antibunching to identify and decode such ...

The particle-like nature of light becomes evident in the photon statistics of fluorescence from single quantum systems as photon antibunching. In multichromophoric systems, exciton diffusion and subsequent annihilation occurs. These processes also yield photon antibunching but cannot be interpreted reliably. Here we develop picosecond time-resolved antibunching to identify and decode such processes. We use this method to measure the true number of chromophores on well-defined multichromophoric DNA-origami structures, and precisely determine the distance-dependent rates of annihilation between excitons. Further, this allows us to measure exciton diffusion in mesoscopic H- and J-type conjugated-polymer aggregates. We distinguish between one-dimensional intra-chain and three-dimensional inter-chain exciton diffusion at different times after excitation and determine the disorder-dependent diffusion lengths. Our method provides a powerful lens through which excitons can be studied at the single-particle level, enabling the rational design of improved excitonic probes such as ultra-bright fluorescent nanoparticles and materials for optoelectronic devices. Photon antibunching typically measures the time-averaged photophysics of multichromophoric nanoparticles. Here, the authors report on time-resolving photon antibunching, allowing the true number of chromophores and exciton diffusion to be measured in DNA origami and conjugated polymer aggregates.



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Details

DokumentenartArtikel
Titel eines Journals oder einer ZeitschriftNature Communications
Verlag:Nature
Ort der Veröffentlichung:BERLIN
Band:12
Nummer des Zeitschriftenheftes oder des Kapitels:1
Seitenbereich:S. 1-10
Datum26 Februar 2021
InstitutionenPhysik > Institut für Experimentelle und Angewandte Physik > Lehrstuhl Professor Lupton > Arbeitsgruppe John Lupton
Identifikationsnummer
WertTyp
10.1038/s41467-021-21474-zDOI
Stichwörter / KeywordsENERGY-TRANSFER; DIFFUSION; PATHWAYS; EMISSION; ANNIHILATION; STATISTICS; MOLECULES; DYNAMICS; EMITTERS
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-463773
Dokumenten-ID46377

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