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

doi:10.17863/cam.56388

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^*

^*Corresponding author for this work

Research output: Working paper › Preprint › Academic

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.

Original language	English
Publisher	University of Cambridge
Number of pages	10
DOIs	https://doi.org/10.17863/cam.56388
Publication status	Published - 17 Aug 2020
Externally published	Yes

Keywords

Spin mixing
Plasmonic nanocavity
Resonant Raman
Photoluminescence
Symmetry breaking

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Breaking the Selection Rules of Spin-Forbidden Molecular Absorption in Plasmonic Nanocavities
Ojambati, O. S., Deacon, W. M., Chikkaraddy, R., Readman, C., Lin, Q., Koczor-Benda, Z., Rosta, E., Scherman, O. A. & Baumberg, J. J., 2020, In: ACS photonics. 7, 9, p. 2337-2342
Research output: Contribution to journal › Article › Academic › peer-review
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Breaking the Selection Rules of Spin-Forbidden Molecular Absorption in Plasmonic Nanocavities
Ojambati, O. S., Deacon, W. M., Chikkaraddy, R., Readman, C., Lin, Q., Koczor-Benda, Z., Rosta, E., Scherman, O. A. & Baumberg, J. J., 11 May 2020, ArXiv.org, 8 p.
Research output: Working paper › Preprint › Academic

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title = "Breaking the Selection Rules of Spin-Forbidden Molecular Absorption in Plasmonic Nanocavities",

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.",

keywords = "Spin mixing, Plasmonic nanocavity, Resonant Raman, Photoluminescence, Symmetry breaking",

author = "Ojambati, \{Oluwafemi S.\} and Deacon, \{William M.\} and Rohit Chikkaraddy and Charlie Readman and Qianqi Lin and Zsuzsanna Koczor-Benda and Edina Rosta and Scherman, \{Oren A.\} and Baumberg, \{Jeremy J.\}",

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AU - Ojambati, Oluwafemi S.

AU - Deacon, William M.

AU - Chikkaraddy, Rohit

AU - Readman, Charlie

AU - Lin, Qianqi

AU - Koczor-Benda, Zsuzsanna

AU - Rosta, Edina

AU - Scherman, Oren A.

AU - Baumberg, Jeremy J.

PY - 2020/8/17

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N2 - 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.

AB - 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.

KW - Spin mixing

KW - Plasmonic nanocavity

KW - Resonant Raman

KW - Photoluminescence

KW - Symmetry breaking

U2 - 10.17863/cam.56388

DO - 10.17863/cam.56388

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

PB - University of Cambridge

ER -

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

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Keywords

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