Exciton-Exciton Annihilation Is Coherently Suppressed in H-Aggregates, but Not in J-Aggregates

Roel Tempelaar*, Thomas L.C. Jansen, Jasper Knoester

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

24 Scopus citations

Abstract

We theoretically demonstrate a strong dependence of the annihilation rate between (singlet) excitons on the sign of dipole-dipole couplings between molecules. For molecular H-aggregates, where this sign is positive, the phase relation of the delocalized two-exciton wave functions causes a destructive interference in the annihilation probability. For J-aggregates, where this sign is negative, the interference is constructive instead; as a result, no such coherent suppression of the annihilation rate occurs. As a consequence, room temperature annihilation rates of typical H- and J-aggregates differ by a factor of ∼3, while an order of magnitude difference is found for low-temperature aggregates with a low degree of disorder. These findings, which explain experimental observations, reveal a fundamental principle underlying exciton-exciton annihilation, with major implications for technological devices and experimental studies involving high excitation densities.

Original languageEnglish (US)
Pages (from-to)6113-6117
Number of pages5
JournalJournal of Physical Chemistry Letters
Volume8
Issue number24
DOIs
StatePublished - Dec 21 2017

ASJC Scopus subject areas

  • Materials Science(all)
  • Physical and Theoretical Chemistry

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