Highly efficient exciton-exciton annihilation in single conjugated polymer chains

Fuente: arXiv
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Main Authors: Fairbairn, Nicola J., Vodianova, Olga, Hedley, Gordon J.
Format: Preprint
Published: 2025
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author Fairbairn, Nicola J.
Vodianova, Olga
Hedley, Gordon J.
author_facet Fairbairn, Nicola J.
Vodianova, Olga
Hedley, Gordon J.
contents The number of excitons that conjugated polymers can support at any one time underpins their optoelectronic performance in light emitting diodes and as laser gain media, as it sets a natural limit on exciton density. Here we have measured the time-resolved photon statistics of single chains of polyfluorene to extract the absolute number of independent emitting sites present and its time dependence. We find that after 100 ps each chain can only support 1 or 2 independent excitons, and that even at the earliest times this number rises only to 4, suggesting a high degree of electronic coupling between chromophores that facilitates efficient exciton-exciton annihilation. In circumstances where a low density of low-energy sites is present, annihilation between them still dominates. The results indicate that achieving high exciton densities in conjugated polymers is difficult, and in applications where it is desirable new strategies should be devised to control exciton-exciton annihilation.
format Preprint
id arxiv_https___arxiv_org_abs_2503_13703
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Highly efficient exciton-exciton annihilation in single conjugated polymer chains
Fairbairn, Nicola J.
Vodianova, Olga
Hedley, Gordon J.
Chemical Physics
Mesoscale and Nanoscale Physics
Materials Science
The number of excitons that conjugated polymers can support at any one time underpins their optoelectronic performance in light emitting diodes and as laser gain media, as it sets a natural limit on exciton density. Here we have measured the time-resolved photon statistics of single chains of polyfluorene to extract the absolute number of independent emitting sites present and its time dependence. We find that after 100 ps each chain can only support 1 or 2 independent excitons, and that even at the earliest times this number rises only to 4, suggesting a high degree of electronic coupling between chromophores that facilitates efficient exciton-exciton annihilation. In circumstances where a low density of low-energy sites is present, annihilation between them still dominates. The results indicate that achieving high exciton densities in conjugated polymers is difficult, and in applications where it is desirable new strategies should be devised to control exciton-exciton annihilation.
title Highly efficient exciton-exciton annihilation in single conjugated polymer chains
topic Chemical Physics
Mesoscale and Nanoscale Physics
Materials Science
url https://arxiv.org/abs/2503.13703