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

Gordon J. Hedley (), Tim Schröder, Florian Steiner, Theresa Eder, Felix J. Hofmann, Sebastian Bange, Dirk Laux, Sigurd Höger, Philip Tinnefeld, John M. Lupton and Jan Vogelsang ()
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Gordon J. Hedley: University of Glasgow
Tim Schröder: Ludwig-Maximilians-Universität München
Florian Steiner: Ludwig-Maximilians-Universität München
Theresa Eder: Universität Regensburg
Felix J. Hofmann: Universität Regensburg
Sebastian Bange: Universität Regensburg
Dirk Laux: Universität Bonn
Sigurd Höger: Universität Bonn
Philip Tinnefeld: Ludwig-Maximilians-Universität München
John M. Lupton: Universität Regensburg
Jan Vogelsang: Universität Regensburg

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: Abstract 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.

Date: 2021
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DOI: 10.1038/s41467-021-21474-z

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