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Breaking the Selection Rules of Spin-Forbidden Molecular Absorption in Plasmonic Nanocavities

Ojambati, OS; Deacon, WM; Chikkaraddy, R; Readman, C; Lin, Q; Koczor-Benda, Z; Rosta, E; ... Baumberg, JJ; + view all (2020) Breaking the Selection Rules of Spin-Forbidden Molecular Absorption in Plasmonic Nanocavities. ACS Photonics , 7 (9) pp. 2337-2342. 10.1021/acsphotonics.0c00732. Green open access

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Abstract

Controlling absorption and emission of organic molecules is crucial for efficient light-emitting diodes, organic solar cells, and single-molecule spectroscopy. Here, a new molecular absorption is activated inside a gold plasmonic nanocavity and found to break selection rules via spin–orbit coupling. Photoluminescence excitation scans reveal absorption from a normally spin-forbidden singlet to triplet state transition, while drastically enhancing the emission rate by several thousand fold. The experimental results are supported by density functional theory, revealing the manipulation of molecular absorption by nearby metallic gold atoms.

Type: Article
Title: Breaking the Selection Rules of Spin-Forbidden Molecular Absorption in Plasmonic Nanocavities
Open access status: An open access version is available from UCL Discovery
DOI: 10.1021/acsphotonics.0c00732
Publisher version: https://doi.org/10.1021/acsphotonics.0c00732
Language: English
Additional information: This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions.
Keywords: spin mixing plasmonic nanocavity resonant Raman photoluminescence symmetry breaking
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Physics and Astronomy
URI: https://discovery.ucl.ac.uk/id/eprint/10111911
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