journal article·2020-09-16Open access

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

Oluwafemi S. Ojambati, William M. Deacon, Rohit Chikkaraddy, Charlie Readman, Qianqi Lin, Zsuzsanna Koczor-Benda, Edina Rosta, Oren A. Scherman, Jeremy J. Baumberg

ACS Photonics· Volume 7· Issue 9

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.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Molecular Junctions and Nanostructures · Quantum and electron transport phenomena · Plasmonic and Surface Plasmon Research

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

NanoPhotonics Centre, Cavendish Laboratory, Department of Physics, University of Cambridge, JJ Thompson Avenue, Cambridge CB3 0HE, United Kingdom

Melville Laboratory for Polymer Synthesis, Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, United Kingdom

Department of Chemistry, King’s College London, 7 Trinity Street, London SE1 1DB, United Kingdom

Department of Physics and Astronomy, University College London, London WC1E 6BT, United Kingdom

Funding

Engineering and Physical Sciences Research Council · Trinity College, University of Cambridge · H2020 Future and Emerging Technologies · H2020 European Research Council · Nederlandse Organisatie voor Wetenschappelijk Onderzoek

References (46)

Show source-provided references
1. Szabo A. · 1996
2. Harris D. C. · 1978
3. 10.1038/nmat436010.1038/nmat4360 ↗
4. 10.1039/C5CS00582E10.1039/C5CS00582E ↗
5. 10.1038/nature1982010.1038/nature19820 ↗
6. 10.1103/RevModPhys.85.124510.1103/RevModPhys.85.1245 ↗
7. McGlynn S. P. · 1969
8. 10.1016/j.ccr.2011.01.04210.1016/j.ccr.2011.01.042 ↗
9. 10.1021/acs.chemrev.7b0006010.1021/acs.chemrev.7b00060 ↗
10. 10.1021/jacs.6b0469210.1021/jacs.6b04692 ↗
11. 10.1021/ja003693s10.1021/ja003693s ↗
12. 10.1002/adma.20170198710.1002/adma.201701987 ↗
13. 10.1073/pnas.061067710410.1073/pnas.0610677104 ↗
14. 10.1038/nchem.98410.1038/nchem.984 ↗
15. 10.1021/acs.jpclett.7b0121510.1021/acs.jpclett.7b01215 ↗
16. 10.1021/acs.jpclett.8b0155610.1021/acs.jpclett.8b01556 ↗
17. 10.1039/C6CS00368K10.1039/C6CS00368K ↗
18. 10.1021/ja508155x10.1021/ja508155x ↗
19. 10.1038/s42004-018-0027-x10.1038/s42004-018-0027-x ↗
20. 10.1103/PhysRevLett.122.05740110.1103/PhysRevLett.122.057401 ↗
21. 10.1126/sciadv.aax448210.1126/sciadv.aax4482 ↗
22. 10.1103/PhysRevApplied.3.01400110.1103/PhysRevApplied.3.014001 ↗
23. 10.1021/jacs.8b0484110.1021/jacs.8b04841 ↗
24. 10.1038/lsa.2016.8010.1038/lsa.2016.80 ↗
25. 10.1038/nnano.2013.9910.1038/nnano.2013.99 ↗
26. 10.1038/nmat262910.1038/nmat2629 ↗
27. 10.1021/jz101426x10.1021/jz101426x ↗
28. 10.1039/C5FD00149H10.1039/C5FD00149H ↗
29. 10.1038/nature0727810.1038/nature07278 ↗
30. 10.1021/jacs.9b0781710.1021/jacs.9b07817 ↗
31. 10.1021/acsphotonics.7b0037410.1021/acsphotonics.7b00374 ↗
32. 10.1021/acs.nanolett.8b0023910.1021/acs.nanolett.8b00239 ↗
33. 10.1038/s41563-019-0290-y10.1038/s41563-019-0290-y ↗
34. 10.1021/acs.nanolett.0c0159310.1021/acs.nanolett.0c01593 ↗
35. 10.1021/jp507199z10.1021/jp507199z ↗
36. 10.1103/PhysRevLett.96.11300210.1103/PhysRevLett.96.113002 ↗
37. 10.1021/acsphotonics.7b0066810.1021/acsphotonics.7b00668 ↗
38. 10.1364/JOSAB.19.00135510.1364/JOSAB.19.001355 ↗
39. 10.1103/PhysRevB.86.03540410.1103/PhysRevB.86.035404 ↗
40. 10.1126/science.aaf630810.1126/science.aaf6308 ↗
41. 10.1021/acsphotonics.6b0010710.1021/acsphotonics.6b00107 ↗
42. 10.1021/acs.nanolett.7b0529710.1021/acs.nanolett.7b05297 ↗
43. 10.1038/s41467-019-13820-z10.1038/s41467-019-13820-z ↗
44. 10.1103/PhysRevLett.103.03740210.1103/PhysRevLett.103.037402 ↗
45. 10.1038/nphoton.2014.8410.1038/nphoton.2014.84 ↗
46. 10.1038/nphoton.2014.22810.1038/nphoton.2014.228 ↗