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Switched "On" Transient Fluorescence Output from a Pulsed-Fuel Molecular Ratchet.


ABSTRACT: We report the synthesis and operation of a molecular energy ratchet that transports a crown ether from solution onto a thread, along the axle, over a fluorophore, and off the other end of the thread back into bulk solution, all in response to a single pulse of a chemical fuel (CCl3CO2H). The fluorophore is a pyrene residue whose fluorescence is normally prevented by photoinduced electron transfer (PET) to a nearby N-methyltriazolium group. However, crown ether binding to the N-methyltriazolium site inhibits the PET, switching on pyrene fluorescence under UV irradiation. Each pulse of fuel results in a single ratchet cycle of transient fluorescence (encompassing threading, transport to the N-methyltriazolium site, and then dethreading), with the onset of the fluorescent time period determined by the amount of fuel in each pulse and the end-point determined by the concentration of the reagents for the disulfide exchange reaction. The system provides a potential alternative signaling approach for artificial molecular machines that read symbols from sequence-encoded molecular tapes.

SUBMITTER: Baluna AS 

PROVIDER: S-EPMC10722508 | biostudies-literature | 2023 Dec

REPOSITORIES: biostudies-literature

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Switched "On" Transient Fluorescence Output from a Pulsed-Fuel Molecular Ratchet.

Baluna Andrei S AS   Dommaschk Marcel M   Groh Burkhard B   Kassem Salma S   Leigh David A DA   Tetlow Daniel J DJ   Thomas Dean D   Varela López Loli L  

Journal of the American Chemical Society 20231204 49


We report the synthesis and operation of a molecular energy ratchet that transports a crown ether from solution onto a thread, along the axle, over a fluorophore, and off the other end of the thread back into bulk solution, all in response to a single pulse of a chemical fuel (CCl<sub>3</sub>CO<sub>2</sub>H). The fluorophore is a pyrene residue whose fluorescence is normally prevented by photoinduced electron transfer (PET) to a nearby <i>N</i>-methyltriazolium group. However, crown ether bindin  ...[more]

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