Resolving ultrafast exciton migration in organic solids at the nanoscale
Open accessAbstract
Effectiveness of molecular-based light harvesting relies on transport of excitons to charge-transfer sites. Measuring exciton migration, however, has been challenging because of the mismatch between nanoscale migration lengths and the diffraction limit. Instead of using bulk substrate quenching methods, here we define quenching boundaries all-optically with sub-diffraction resolution, thus characterizing spatiotemporal exciton migration on its native nanometre and picosecond scales. By transforming stimulated emission depletion microscopy into a time-resolved ultrafast approach, we measure a 16-nm migration length in poly(2,5-di(hexyloxy)cyanoterephthalylidene) conjugated polymer films. Combined with Monte Carlo exciton hopping simulations, we show that migration in these films is essentially diffusive because intrinsic chromophore energetic disorder is comparable to chromophore inhomogeneous broadening. Our approach will enable previously unattainable correlation of local material structure to exciton migration character, applicable not only to photovoltaic or display-destined organic semiconductors but also to explaining the quintessential exciton migration exhibited in photosynthesis.
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The 2D diffusion length in microtubules is comparable to that observed in some photosynthetic complexes and organic photovoltaic devices.
“Stern–Volmer analysis revealed that the 2D diffusion length of tryptophan photoexcitation in microtubules is comparable to that observed in some photosynthetic complexes23−25 and organic photovoltaic devices.45−47”
From Electronic energy migration in microtubules (2023) · cites this paper as [45]
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References 39 · Cited by 52
Research works printed but not linked: 2
- [5]5. Holzapfel, C. On statistics of timetoamplitude converter systems in photon counting devices. Review of Scientific Instruments 45, 894-896. issn : 0034-6748, 1089-7623 (July 1, 1974).
- [12]12. Lakowicz, J. R. Principles of Fluorescence Spectroscopy isbn : 978-0-387-46312-4 (Springer Science & Business Media, 2007).
- Authors
- Penwell, S. B., Ginsberg, L. D. S., Noriega, R., & Ginsberg, N. S.
- Affiliations
- University of California, Berkeley (US)
- Lawrence Berkeley National Laboratory (US)
- Corresponding author
- Ginsberg, Naomi S.
- Venue
- Nature Materials
- Published
- 2017-09-18
- Volume
- 16
- Issue
- 11
- Pages
- 1136-1141
- ISSN
- 1476-1122 (ISSN-L)
- 1476-4660
- OpenAlex
- W2655429086
- Cited by
- 52
- References
- 39
- Citations by year
- 2026: 2 · 2025: 2 · 2024: 4 · 2023: 7 · 2022: 3 · 2021: 8 · 2020: 13 · 2019: 7 · 2018: 6
- FWCI
- 2.96
- Type
- journal article
- Language
- en
- Open access
- green
- arxiv.org
- Locations
- Nature Materials (publishedVersion)
- PubMed (publishedVersion)
- arXiv (Cornell University) (submittedVersion)
- arXiv (Cornell University)
- Topics
- Physical Sciences › Engineering › Electrical and Electronic Engineering › Organic Electronics and Photovoltaics
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Spectroscopy and Quantum Chemical Studies
- Physical Sciences › Chemistry › Physical and Theoretical Chemistry › Photochemistry and Electron Transfer Studies
- Keywords
- exciton migration, organic semiconductors, conjugated polymers, STED microscopy, sub-diffraction resolution, exciton hopping, diffusive transport, energetic disorder, inhomogeneous broadening, light harvesting, photosynthesis, Monte Carlo simulation
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