Optoplasmonic characterisation of reversible disulfide interactions at single thiol sites in the attomolar regime

Serge Vincent (), Sivaraman Subramanian and Frank Vollmer ()
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Serge Vincent: University of Exeter
Sivaraman Subramanian: University of Exeter
Frank Vollmer: University of Exeter

Nature Communications, 2020, vol. 11, issue 1, 1-8

Abstract: Abstract Probing individual chemical reactions is key to mapping reaction pathways. Trace analysis of sub-kDa reactants and products is obfuscated by labels, however, as reaction kinetics are inevitably perturbed. The thiol-disulfide exchange reaction is of specific interest as it has many applications in nanotechnology and in nature. Redox cycling of single thiols and disulfides has been unresolvable due to a number of technological limitations, such as an inability to discriminate the leaving group. Here, we demonstrate detection of single-molecule thiol-disulfide exchange using a label-free optoplasmonic sensor. We quantify repeated reactions between sub-kDa thiolated species in real time and at concentrations down to 100’s of attomolar. A unique sensing modality is featured in our measurements, enabling the observation of single disulfide reaction kinetics and pathways on a plasmonic nanoparticle surface. Our technique paves the way towards characterising molecules in terms of their charge, oxidation state, and chirality via optoplasmonics.

Date: 2020
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DOI: 10.1038/s41467-020-15822-8

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