Picosecond time-resolved photon antibunching measures nanoscale exciton motion and the true number of chromophores
Open accessAbstract
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.
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Depending on their aggregation states (i.e., J-, H-, or random aggregates), CP aggregates that contain tens of CP chains showed fluorescence emission from a different number of the chromophores, in some cases only from a few chromophores.
“Depending on their aggregation states (i.e., J-, H-, or random aggregates), CP aggregates that contain tens of CP chains showed fluorescence emission from a different number of the chromophores, in some cases only from a few chromophores.165−167”
From The Pursuit of Shortwave Infrared-Emitting Nanoparticles with Bright Fluorescence through Molecular Design and Excited-State Engineering of Molecular Aggregates (2022) · cites this paper as [167]
In Results, under “Exciton diffusion in conjugated polymer aggregates” (page not provided), the paper compares H- and J-type aggregates and reports different time-dependent numbers of independently emitting chromophores. It reports about 54 chains per H-type aggregate but about 9 per J-type aggregate. It does not study a separate random-aggregate class or establish that aggregates containing tens of chains emitted from only a few chromophores. (LLM, conf=0.84)
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References 46 · Cited by 32
- Authors
- Hedley, G. J., Schröder, T., Steiner, F., Eder, T., Hofmann, F. J., Bange, S., Laux, D., Höger, S., Tinnefeld, P., Lupton, J. M., & Vogelsang, J.
- Affiliations
- University of Glasgow (GB)
- Center for NanoScience (DE)
- University of Regensburg (DE)
- University of Bonn (DE)
- Corresponding author
- Hedley, Gordon J.
- Vogelsang, Jan
- Venue
- Nature Communications
- Published
- 2021-02-26
- Volume
- 12
- Issue
- 1
- Pages
- 1327-1327
- ISSN
- 2041-1723 (ISSN-L)
- PMC
- PMC7910429
- OpenAlex
- W3087824261
- Cited by
- 32
- References
- 46
- Citations by year
- 2026: 4 · 2025: 8 · 2024: 4 · 2023: 4 · 2022: 7 · 2021: 5
- FWCI
- 2.18
- Type
- journal article
- Language
- en
- Open access
- gold
- doi.org
- Locations
- Nature Communications (publishedVersion, cc-by)
- PubMed Central (publishedVersion, cc-by)
- PubMed (publishedVersion)
- ENLIGHTEN (Jurnal Bimbingan dan Konseling Islam) (acceptedVersion, cc-by-sa)
- arXiv (Cornell University) (submittedVersion)
- DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion, cc-by-sa)
- arXiv (Cornell University)
- Funders
- European Commission (314695032, HORIZON2020, 737089)
- Deutsche Forschungsgemeinschaft (390776260, 2089/1390776260, EXC‐2089, EXC 2089/1390776260, EXC 2089/1, project B03), 319559986, 314695032)
- Engineering and Physical Sciences Research Council (EP/V004921/1, EP/V048805/1)
- Topics
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Semiconductor Quantum Structures and Devices
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Spectroscopy and Quantum Chemical Studies
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Strong Light-Matter Interactions
- Keywords
- photon antibunching, exciton diffusion, exciton-exciton annihilation, DNA origami
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