Luminescent radical molecules with addressable high-spin states: combination of optical and spin resonance spectroscopies reveals unique mechanism Sebastian Gorgon 1,2 , Jeannine Grüne 3 , William Myers 2 , Giacomo Londi 4 , Andreas Sperlich 3 , Vladimir Dyakonov 3 , David Beljonne 5 , Yoann Olivier 4 , Feng Li 6 , Richard Friend 1 , Emrys Evans 7 1 University of Cambridge,UK, 2 University of Oxford, UK, 3 University of Würzburg,Germany, 4 University of Namur, Belgium, 5 University of Mons, Belgium, 6 Jilin University, China, 7 Swansea University, UK Molecules present a versatile new platform for quantum information science. 1 They offer potential for chemical tunability through established synthetic approaches and are candidates for sensing and computation applications. Here we present a new molecular architecture that enables the three critical functions: control of spin state initialisation, manipulation and read-out. Creation of robust spin-optical interfaces is key to harnessing the quantum resources of materials, but all prior organic candidates are non-luminescent. 2 Here we report the first organic molecules displaying both efficient luminescence and near-unity generation yield of high-spin multiplicity excited states. We attach a tris(2,4,6- trichlorophenyl) methyl-carbazole emissive radical (TTM-1Cz) to anthracene to achieve energy resonance between the excited radical doublet and anthracene triplet levels. Using a combination of time-resolved optical and spin resonance spectroscopies we track the wavefunction evolution and reveal a unique mechanism. 3 We observe the doublet photoexcitation delocalise onto the linked acene within a few picoseconds and subsequently evolve to a pure spin quartet state of mixed radical-triplet character. The resulting high-spin state is coherently addressable even at 295 K. Through its ability to readily reform the emissive doublet state after microwave manipulation this system presents a new type of spin-optical interface. Our approach simultaneously supports a high efficiency of initialisation, spin manipulationsat room temperature and light-based read-out. This advance creates a platform for emerging quantum technologies. References 1. Wasielewski, M.R., Forbes, M.D.E., Frank, N.L.et al.Exploiting chemistry and molecular systems for quantum information science.Nat Rev Chem 4 , 490–504 (2020). https://doi.org/10.1038/s41570-020-0200-5 2. Quintes, T., Mayländer, M. & Richert, S. Properties and applications of photoexcited chromophore–radical systems.Nat Rev Chem(2023). https://doi.org/10.1038/s41570-022-00453-yGorgonet al.,(2023),under review
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