Electrochemical Fluorescence Switching in Rhodamine-Ferrocene Dyads: Spatiotemporal Control in Biomimetic Membranes
Abstract
The electrochemical control of fluorescence has been extensively developed in homogeneous media, yet its implementation within electrically insulating lipid bilayers remains largely unexplored. Here we establish that an electrochemically gated fluorescence switch can be implemented in individual giant unilamellar vesicles using a rhodamine-ferrocene dyad that modulates emission through redox-controlled photoinduced electron transfer. A membraneanchored derivative enables direct visualization of reversible fluorescence activation under electrochemical bias. Remarkably, the switching is strictly leaflet-selective and occurs only for dyads exposed to the electrode interface, highlighting the insulating nature of lipid bilayers. Furthermore, membrane surface charge critically governs the switching efficiency and induces pronounced kinetic asymmetry between oxidation and reduction processes, revealing the key role of interfacial electrostatic interactions in redox-controlled emission. These results establish electrochemical fluorescence modulation in membranes as a spatially and electrostatically gated interfacial process and define general principles for redox-responsive probes operating in soft interfaces, such as lipid membranes.
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BibTeX
@article{jiang2026electrochemical,
title = {{Electrochemical Fluorescence Switching in Rhodamine-Ferrocene Dyads: Spatiotemporal Control in Biomimetic Membranes}},
author = {Ning Jiang and Lorenzo Meneghelli and Niccolo Dipace and Carolina Chieffo and Bixente Carré and Ambre Etcheverria and Manuel Pedrón and Manon Guille-Collignon and Frédéric Lemaître and Frédéric Labat and Ilaria Ciofini and Blaise Dumat and Jean-Maurice Mallet and Jérôme Delacotte and Eric Labbé and Olivier Buriez},
journal = {Journal of the American Chemical Society},
year = {2026},
month = sep,
doi = {10.1021/jacs.6c07688},
url = {https://hal.science/hal-05733926v1},
note = {CC BY 4.0},
}
RIS
TY - JOUR
TI - Electrochemical Fluorescence Switching in Rhodamine-Ferrocene Dyads: Spatiotemporal Control in Biomimetic Membranes
AU - Ning Jiang
AU - Lorenzo Meneghelli
AU - Niccolo Dipace
AU - Carolina Chieffo
AU - Bixente Carré
AU - Ambre Etcheverria
AU - Manuel Pedrón
AU - Manon Guille-Collignon
AU - Frédéric Lemaître
AU - Frédéric Labat
AU - Ilaria Ciofini
AU - Blaise Dumat
AU - Jean-Maurice Mallet
AU - Jérôme Delacotte
AU - Eric Labbé
AU - Olivier Buriez
PY - 2026
DA - 2026/09/01
JO - Journal of the American Chemical Society
DO - 10.1021/jacs.6c07688
UR - https://hal.science/hal-05733926v1
AB - The electrochemical control of fluorescence has been extensively developed in homogeneous media, yet its implementation within electrically insulating lipid bilayers remains largely unexplored. Here we establish that an electrochemically gated fluorescence switch can be implemented in individual giant unilamellar vesicles using a rhodamine-ferrocene dyad that modulates emission through redox-controlled photoinduced electron transfer. A membraneanchored derivative enables direct visualization of reversible fluorescence activation under electrochemical bias. Remarkably, the switching is strictly leaflet-selective and occurs only for dyads exposed to the electrode interface, highlighting the insulating nature of lipid bilayers. Furthermore, membrane surface charge critically governs the switching efficiency and induces pronounced kinetic asymmetry between oxidation and reduction processes, revealing the key role of interfacial electrostatic interactions in redox-controlled emission. These results establish electrochemical fluorescence modulation in membranes as a spatially and electrostatically gated interfacial process and define general principles for redox-responsive probes operating in soft interfaces, such as lipid membranes.
SN - 0002-7863
SN - 1520-5126
ER -