Coulombic control of charge transfer in radicals with quartet recycling luminescence

Excitons in organic materials are emerging as an attractive platform for tunable quantum technologies. Structures with near-degenerate doublet and triplet excitations in linked trityl radical, acene and carbazole units can host quartet states. These high spin states can be coherently manipulated, and later decay radiatively via the radical doublet transition. However, this requires controlling the deexcitation pathways of all metastable states. Here we establish design rules for efficient quartet generation and recycling to luminescence, using different connection arrangements of the molecular units. We discover that electronic coupling strength between these units dictates quartet formation and delayed emission yields, particularly through a Coulombically tuned acene-radical charge transfer state. This state acts as a source of non-radiative decay when acene-radical separation is small, but facilitates reversible doublet-quartet interconversion when acene-radical separation is large. Using these rules we report a material with 55% luminescence yield, where 94% of emitting excitons are recycled from the quartet with a 1.0 μs lifetime. This reveals the central role of molecular topology in luminescent quantum materials.

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Publication Details

Journal
Nature Communications
Published
2026-05-22
DOI
https://doi.org/10.1038/s41467-026-72487-5
Primary Topic
Luminescence and Fluorescent Materials
Type
article
Field-Weighted Citation Impact
0.00

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article

Coulombic control of charge transfer in radicals with quartet recycling luminescence

James D. Green, Timothy J. H. Hele, Weixuan Zeng, Lars van Turnhout et al.
Nature Communications
Luminescence and Fluorescent Materials
article

Coulombic control of charge transfer in radicals with quartet recycling luminescence

James D. Green, Timothy J. H. Hele, Weixuan Zeng, Lars van Turnhout, Petri Murto, William K. Myers, Giacomo Londi, F F Li, Shilong Yu, Laura Brown, Sergiu Petrusca, Konstantina Armadorou, David Beljonne, Richard H. Friend, Hugo Bronstein, Lujo Matasovic, Yoann Olivier, Wenzhao Wang, Sebastian Gorgon, Avik Bhanja
article en

Abstract

Excitons in organic materials are emerging as an attractive platform for tunable quantum technologies. Structures with near-degenerate doublet and triplet excitations in linked trityl radical, acene and carbazole units can host quartet states. These high spin states can be coherently manipulated, and later decay radiatively via the radical doublet transition. However, this requires controlling the deexcitation pathways of all metastable states. Here we establish design rules for efficient quartet generation and recycling to luminescence, using different connection arrangements of the molecular units. We discover that electronic coupling strength between these units dictates quartet formation and delayed emission yields, particularly through a Coulombically tuned acene-radical charge transfer state. This state acts as a source of non-radiative decay when acene-radical separation is small, but facilitates reversible doublet-quartet interconversion when acene-radical separation is large. Using these rules we report a material with 55% luminescence yield, where 94% of emitting excitons are recycled from the quartet with a 1.0 μs lifetime. This reveals the central role of molecular topology in luminescent quantum materials.

Nature Communications
University of Pisa (IT), University of Mons (BE), University of Namur (BE), Jilin University (CN), University of Cambridge (GB), University of Oxford (GB), Bridge University (SS), State Key Laboratory of Supramolecular Structure and Materials, University College London (GB), The University of Tokyo (JP), Aalto University (FI)
European Commission
Openalex Percentile: Top 11%
Luminescence and Fluorescent Materials
DOIOpen Access PDFOpenAlex
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