Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 115, Issue 20, Pages 5077-5082Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1718868115
Keywords
organic semiconductors; exchange coupling; triplet excitons; singlet fission; organic spintronics
Categories
Funding
- HFML-RU/FOM of the European Magnetic Field Laboratory (EMFL)
- LNCMI-CNRS of the European Magnetic Field Laboratory (EMFL)
- EPSRC (United Kingdom) via EMFL Grants [EP/N01085X/1, NS/A000060/1]
- EPSRC (United Kingdom) [EP/M005143/1]
- Gates-Cambridge Scholarship
- Winton Scholarship
- Labex [ANR-10-LABX-0039-PALM]
- ANR SPINEX
- DFG [SPP-1601 (Bi-464/10-2)]
- EPSRC [EP/M006360/1, EP/N01085X/1, NS/A000060/1] Funding Source: UKRI
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From organic electronics to biological systems, understanding the role of intermolecular interactions between spin pairs is a key challenge. Here we show how such pairs can be selectively addressed with combined spin and optical sensitivity. We demonstrate this for bound pairs of spin-triplet excitations formed by singlet fission, with direct applicability across a wide range of synthetic and biological systems. We show that the site sensitivity of exchange coupling allows distinct triplet pairs to be resonantly addressed at different magnetic fields, tuning them between optically bright singlet (S = 0) and dark triplet quintet (S = 1, 2) configurations: This induces narrow holes in a broad optical emission spectrum, uncovering exchange-specific luminescence. Using fields up to 60 T, we identify three distinct triplet-pair sites, with exchange couplings varying over an order of magnitude (0.3-5 meV), each with its own luminescence spectrum, coexisting in a single material. Our results reveal how site selectivity can be achieved for organic spin pairs in a broad range of systems.
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