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Reversible spin-optical interface in luminescent organic radicals
,
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 ,
Emrys Evans
Nature, Volume: 620, Issue: 7974, Pages: 538 - 544
Swansea University Author:
Emrys Evans
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DOI (Published version): 10.1038/s41586-023-06222-1
Abstract
Molecules present a versatile platform for quantum information science and are candidates for sensing and computation applications. Robust spin-optical interfaces are key to harnessing the quantum resources of materials. To date, carbon-based candidates have been non-luminescent, which prevents opti...
| Published in: | Nature |
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| ISSN: | 0028-0836 1476-4687 |
| Published: |
Springer Science and Business Media LLC
2023
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| Online Access: |
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| URI: | https://cronfa.swan.ac.uk/Record/cronfa63993 |
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| Abstract: |
Molecules present a versatile platform for quantum information science and are candidates for sensing and computation applications. Robust spin-optical interfaces are key to harnessing the quantum resources of materials. To date, carbon-based candidates have been non-luminescent, 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. |
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| Keywords: |
Chemical physics, excited states, molecular electronics, quantum physics |
| College: |
Faculty of Science and Engineering |
| Funders: |
European Research Council, European Union’s Horizon 2020 research and innovation programme grant agreement no. 101020167, Engineering and Physical Sciences Research Council (EPSRC) Cambridge NanoDTC, no. EP/S022953/1, Simons Foundation, grant no. 601946, Royal Society, University Research Fellowship, grant no. URF\R1\201300, Leverhulme Trust Early Career Fellowship, grant no. ECF-2019-054, EPSRC grant no. EP/W018519/1, National Natural Science Foundation of China, grant no. 51925303, Deutsche Forschungsgemeinschaft, Research Training School ‘Molecular biradicals: Structure, properties and reactivity’ (no. GRK2112), Bavarian Ministry of the Environment and Consumer Protection, the Bavarian Network ‘Solar Technologies Go Hybrid’, John Fell OUP Research Fund, grant no. 0007019, EPSRC, grant nos. EP/V036408/1 and EP/L011972/1, Department of Chemistry, University of Oxford, Fonds de la Recherche Scientifiques de Belgique (F.R.S.-FNRS), grant no. 2.5020.11, Walloon Region, grant no. 1117545, Fonds pour la formation à la Recherche dans l’Industrie et dans l’Agriculture of the F.R.S.-F.N.R.S., Fonds de la Recherche Scientifique-FNRS, grant no. F.4534.21 (MIS-IMAGINE), Ministerio de Ciencia e Innovación of Spain, project no. PID2019-109555GB-I00, and Eusko Jaurlaritza/Basque Government, project nos. PIBA19-0004 and 2019-CIEN-000092-01, Consortium des Équipements de Calcul Intensif and the Tier-1 supercomputer of Fedération Wallonie-Bruxelles, FNRS, Donostia International Physics Centre and Gipuzkoa’s council joint programme Women and Science, DIPC Computer Centre. |
| Issue: |
7974 |
| Start Page: |
538 |
| End Page: |
544 |