Breaking the Selection Rules of Spin-Forbidden Molecular Absorption in Plasmonic Nanocavities
Accepted version
Peer-reviewed
Repository URI
Repository DOI
Change log
Authors
Ojambati, OS https://orcid.org/0000-0002-8028-4386
Deacon, WM
Chikkaraddy, R https://orcid.org/0000-0002-3840-4188
Readman, C
Lin, Q
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.
Description
Keywords
spin mixing, plasmonic nanocavity, resonant Raman, photoluminescence, symmetry breaking
Journal Title
ACS Photonics
Conference Name
Journal ISSN
2330-4022
2330-4022
2330-4022
Volume Title
7
Publisher
American Chemical Society (ACS)
Publisher DOI
Rights
All rights reserved
Sponsorship
Engineering and Physical Sciences Research Council (EP/L027151/1)
Netherlands Organisation for Scientific Research (NWO) (680-50-1530)
Engineering and Physical Sciences Research Council (EP/G060649/1)
Netherlands Organisation for Scientific Research (NWO) (680-50-1530)
Engineering and Physical Sciences Research Council (EP/G060649/1)