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Spatial Correlations Drive Long-Range Transport and Trapping of Excitons in Single H-Aggregates : Experiment and Theory

Title data

Carta, Alberto ; Wittmann, Bernd ; Kreger, Klaus ; Schmidt, Hans-Werner ; Jansen, Thomas L. C. ; Hildner, Richard:
Spatial Correlations Drive Long-Range Transport and Trapping of Excitons in Single H-Aggregates : Experiment and Theory.
In: The Journal of Physical Chemistry Letters. Vol. 15 (2024) Issue 10 . - pp. 2697-2707.
ISSN 1948-7185
DOI: https://doi.org/10.1021/acs.jpclett.3c03586

Official URL: Volltext

Project information

Project financing: Bayerisches Staatsministerium für Wissenschaft, Forschung und Kunst
Solar Technologies Go Hybrid

Abstract in another language

Describing long-range energy transport is a crucial step, both toward deepening our knowledge on natural light-harvesting systems and toward developing novel photoactive materials. Here, we combine experiment and theory to resolve and reproduce energy transport on pico- to nanosecond time scales in single H-type supramolecular nanofibers based on carbonyl-bridged triarylamines (CBT). Each nanofiber shows energy transport dynamics over long distances up to ∼1 μm, despite exciton trapping at specific positions along the nanofibers. Using a minimal Frenkel exciton model including disorder, we demonstrate that spatial correlations in the normally distributed site energies are crucial to reproduce the experimental data. In particular, we can observe the long-range and subdiffusive nature of the exciton dynamics as well as the trapping behavior of excitons in specific locations of the nanofiber. This trapping behavior introduces a net directionality or asymmetry in the exciton dynamics as observed experimentally. Describing long-range energy transport is a crucial step, both toward deepening our knowledge on natural light-harvesting systems and toward developing novel photoactive materials. Here, we combine experiment and theory to resolve and reproduce energy transport on pico- to nanosecond time scales in single H-type supramolecular nanofibers based on carbonyl-bridged triarylamines (CBT). Each nanofiber shows energy transport dynamics over long distances up to ∼1 μm, despite exciton trapping at specific positions along the nanofibers. Using a minimal Frenkel exciton model including disorder, we demonstrate that spatial correlations in the normally distributed site energies are crucial to reproduce the experimental data. In particular, we can observe the long-range and subdiffusive nature of the exciton dynamics as well as the trapping behavior of excitons in specific locations of the nanofiber. This trapping behavior introduces a net directionality or asymmetry in the exciton dynamics as observed experimentally.

Further data

Item Type: Article in a journal
Refereed: Yes
Institutions of the University: Faculties > Faculty of Biology, Chemistry and Earth Sciences > Department of Chemistry > Former Professors > Chair Macromolecular Chemistry I - Univ.-Prof. Dr. Hans-Werner Schmidt
Profile Fields > Advanced Fields > Polymer and Colloid Science
Result of work at the UBT: No
DDC Subjects: 500 Science > 500 Natural sciences
500 Science > 530 Physics
500 Science > 540 Chemistry
Date Deposited: 10 Jun 2024 07:54
Last Modified: 10 Jun 2024 07:55
URI: https://eref.uni-bayreuth.de/id/eprint/89693