Outsourcing Intersystem Crossing without Heavy Atoms: Energy Transfer Dynamics in PyridoneBODIPY-C60Complexes

Rachel K. Swedin, Andrew T. Healy, Jacob W. Schaffner, Ilya A. Kuzmin, Yuriy V. Zatsikha, Victor N. Nemykin, David A. Blank

Research output: Contribution to journalArticlepeer-review

6 Scopus citations

Abstract

The excited state dynamics in two fully characterized pyridoneBODIPY-fullerene complexes were investigated using time-resolved spectroscopy. Photoexcitation was initially localized on the pyridoneBODIPY chromophore. The energy was rapidly transferred to the fullerene, which subsequently underwent ISC to form a triplet state and returned the energy to the pyridoneBODIPY via triplet-triplet energy transfer. This ping-pong energy transfer mechanism resulted in efficient (>85%) overall conversion of the excited state pyridoneBODIPY constituent despite a complete lack of ISC in the pyridoneBODIPY in the absence of the fullerene partner. The small difference in attachment chemistry for the fullerene did not impact the initial singlet energy transfer. However, the N-methylpyrrolidine bridge did slow both the triplet-triplet energy transfer and the ultimate relaxation rate of the final triplet state when compared to an isoxazole-based bridge. The rates of each step were quantified, and computational predictions were used to complement the proposed mechanism and energetics. The result demonstrated efficient triplet sensitization of a strong chromophore that lacks significant spin-orbit coupling.

Original languageEnglish (US)
Pages (from-to)8845-8850
Number of pages6
JournalJournal of Physical Chemistry Letters
Volume13
Issue number38
DOIs
StatePublished - Sep 29 2022

Bibliographical note

Funding Information:
This work was supported by the Minnesota Supercomputing Institute and the National Science Foundation under Grant CHE-2153081.

Publisher Copyright:
© 2022 American Chemical Society.

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