Reversible spin-optical interface in luminescent organic radicals

Sebastian Gorgon (), Kuo Lv, Jeannine Grüne, Bluebell H. Drummond, William K. Myers, Giacomo Londi, Gaetano Ricci, Danillo Valverde, Claire Tonnelé, Petri Murto, Alexander S. Romanov, David Casanova, Vladimir Dyakonov, Andreas Sperlich, David Beljonne, Yoann Olivier, Feng Li, Richard H. Friend () and Emrys W. Evans ()
Additional contact information
Sebastian Gorgon: University of Cambridge
Kuo Lv: Jilin University
Jeannine Grüne: University of Würzburg
Bluebell H. Drummond: University of Cambridge
William K. Myers: University of Oxford, Inorganic Chemistry Laboratory
Giacomo Londi: University of Namur
Gaetano Ricci: University of Namur
Danillo Valverde: University of Namur
Claire Tonnelé: Donostia International Physics Centre
Petri Murto: University of Cambridge
Alexander S. Romanov: University of Manchester
David Casanova: Donostia International Physics Centre
Vladimir Dyakonov: University of Würzburg
Andreas Sperlich: University of Würzburg
David Beljonne: University of Mons
Yoann Olivier: University of Namur
Feng Li: Jilin University
Richard H. Friend: University of Cambridge
Emrys W. Evans: Swansea University

Nature, 2023, vol. 620, issue 7974, 538-544

Abstract: Abstract Molecules present a versatile platform for quantum information science1,2 and are candidates for sensing and computation applications3,4. Robust spin-optical interfaces are key to harnessing the quantum resources of materials5. To date, carbon-based candidates have been non-luminescent6,7, which prevents optical readout via emission. Here we report organic molecules showing both efficient luminescence and near-unity generation yield of excited states with spin multiplicity S > 1. This was achieved by designing an energy resonance between emissive doublet and triplet levels, here on covalently coupled tris(2,4,6-trichlorophenyl) methyl-carbazole radicals and anthracene. We observed that the doublet photoexcitation delocalized onto the linked acene within a few picoseconds and subsequently evolved to a pure high-spin state (quartet for monoradical, quintet for biradical) of mixed radical–triplet character near 1.8 eV. These high-spin states are coherently addressable with microwaves even at 295 K, with optical readout enabled by reverse intersystem crossing to emissive states. Furthermore, for the biradical, on return to the ground state the previously uncorrelated radical spins either side of the anthracene shows strong spin correlation. Our approach simultaneously supports a high efficiency of initialization, spin manipulations and light-based readout at room temperature. The integration of luminescence and high-spin states creates an organic materials platform for emerging quantum technologies.

Date: 2023
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DOI: 10.1038/s41586-023-06222-1

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