Luciferase-free Luciferin Electrochemiluminescence

Luciferin is one of Nature's most widespread luminophores, and enzymes that catalyze luciferin luminescence are the basis of successful commercial “glow” assays for gene expression and metabolic ATP formation. Herein we report an electrochemical method to promote firefly's luciferin lumine...

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Main Authors: Belotti, Mattia, El-Tahawy, M.M.T., Yu, L.J., Russell, I.C., Darwish, Nadim, Coote, M.L., Garavelli, M., Ciampi, Simone
Format: Journal Article
Language:English
Published: WILEY-V C H VERLAG GMBH 2022
Subjects:
Online Access:http://purl.org/au-research/grants/arc/DP190100735
http://hdl.handle.net/20.500.11937/90478
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author Belotti, Mattia
El-Tahawy, M.M.T.
Yu, L.J.
Russell, I.C.
Darwish, Nadim
Coote, M.L.
Garavelli, M.
Ciampi, Simone
author_facet Belotti, Mattia
El-Tahawy, M.M.T.
Yu, L.J.
Russell, I.C.
Darwish, Nadim
Coote, M.L.
Garavelli, M.
Ciampi, Simone
author_sort Belotti, Mattia
building Curtin Institutional Repository
collection Online Access
description Luciferin is one of Nature's most widespread luminophores, and enzymes that catalyze luciferin luminescence are the basis of successful commercial “glow” assays for gene expression and metabolic ATP formation. Herein we report an electrochemical method to promote firefly's luciferin luminescence in the absence of its natural biocatalyst—luciferase. We have gained experimental and computational insights on the mechanism of the enzyme-free luciferin electrochemiluminescence, demonstrated its spectral tuning from green to red by means of electrolyte engineering, proven that the colour change does not require, as still debated, a keto/enol isomerization of the light emitter, and gained evidence of the electrostatic-assisted stabilization of the charge-transfer excited state by double layer electric fields. Luciferin's electrochemiluminescence, as well as the in situ generation of fluorescent oxyluciferin, are applied towards an optical measurement of diffusion coefficients.
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institution Curtin University Malaysia
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spelling curtin-20.500.11937-904782023-03-20T04:50:06Z Luciferase-free Luciferin Electrochemiluminescence Belotti, Mattia El-Tahawy, M.M.T. Yu, L.J. Russell, I.C. Darwish, Nadim Coote, M.L. Garavelli, M. Ciampi, Simone Science & Technology Physical Sciences Chemistry, Multidisciplinary Chemistry Electrochemiluminescence Electrochemistry Electrostatic Interactions Profluorescence Quantum Chemistry ELECTRICAL DOUBLE-LAYER FIREFLY LUCIFERIN SPECTRAL DISTRIBUTION BIOLUMINESCENCE CHEMILUMINESCENCE MECHANISM MODULATION LIGHT LUMINESCENCE OXIDATION Luciferin is one of Nature's most widespread luminophores, and enzymes that catalyze luciferin luminescence are the basis of successful commercial “glow” assays for gene expression and metabolic ATP formation. Herein we report an electrochemical method to promote firefly's luciferin luminescence in the absence of its natural biocatalyst—luciferase. We have gained experimental and computational insights on the mechanism of the enzyme-free luciferin electrochemiluminescence, demonstrated its spectral tuning from green to red by means of electrolyte engineering, proven that the colour change does not require, as still debated, a keto/enol isomerization of the light emitter, and gained evidence of the electrostatic-assisted stabilization of the charge-transfer excited state by double layer electric fields. Luciferin's electrochemiluminescence, as well as the in situ generation of fluorescent oxyluciferin, are applied towards an optical measurement of diffusion coefficients. 2022 Journal Article http://hdl.handle.net/20.500.11937/90478 10.1002/anie.202209670 English http://purl.org/au-research/grants/arc/DP190100735 http://purl.org/au-research/grants/arc/FT190100148 http://purl.org/au-research/grants/arc/FL170100041 http://purl.org/au-research/grants/arc/CE140100012 http://creativecommons.org/licenses/by-nc-nd/4.0/ WILEY-V C H VERLAG GMBH fulltext
spellingShingle Science & Technology
Physical Sciences
Chemistry, Multidisciplinary
Chemistry
Electrochemiluminescence
Electrochemistry
Electrostatic Interactions
Profluorescence
Quantum Chemistry
ELECTRICAL DOUBLE-LAYER
FIREFLY LUCIFERIN
SPECTRAL DISTRIBUTION
BIOLUMINESCENCE
CHEMILUMINESCENCE
MECHANISM
MODULATION
LIGHT
LUMINESCENCE
OXIDATION
Belotti, Mattia
El-Tahawy, M.M.T.
Yu, L.J.
Russell, I.C.
Darwish, Nadim
Coote, M.L.
Garavelli, M.
Ciampi, Simone
Luciferase-free Luciferin Electrochemiluminescence
title Luciferase-free Luciferin Electrochemiluminescence
title_full Luciferase-free Luciferin Electrochemiluminescence
title_fullStr Luciferase-free Luciferin Electrochemiluminescence
title_full_unstemmed Luciferase-free Luciferin Electrochemiluminescence
title_short Luciferase-free Luciferin Electrochemiluminescence
title_sort luciferase-free luciferin electrochemiluminescence
topic Science & Technology
Physical Sciences
Chemistry, Multidisciplinary
Chemistry
Electrochemiluminescence
Electrochemistry
Electrostatic Interactions
Profluorescence
Quantum Chemistry
ELECTRICAL DOUBLE-LAYER
FIREFLY LUCIFERIN
SPECTRAL DISTRIBUTION
BIOLUMINESCENCE
CHEMILUMINESCENCE
MECHANISM
MODULATION
LIGHT
LUMINESCENCE
OXIDATION
url http://purl.org/au-research/grants/arc/DP190100735
http://purl.org/au-research/grants/arc/DP190100735
http://purl.org/au-research/grants/arc/DP190100735
http://purl.org/au-research/grants/arc/DP190100735
http://hdl.handle.net/20.500.11937/90478