Quantum mechanical tunnelling probes with redox cycling for ultra‐sensitive detection of biomolecules
File(s)
Accepted version
Author(s)
Type
Journal Article
Abstract
Quantum mechanical tunnelling sensors (QMTs) have emerged as a promising technology for next-generation single-molecule detection. Furthermore, QMT sensors can be combined with redox species resulting in repeated oxidation and reduction (redox cycling).. We developed robust QMT probes with electrode gap distances below 2 nm. Using the generator-collector (GC) mode, we verified that redox cycling of the ferrocyanide/ferricyanide (Fe(CN)63−/4−) couple occurs both in the tunnelling regime and on the electrode surface. Our findings indicated that the current enhancement is affected by both the gap distance and surface modifications of the probes. These QMT probes exhibited remarkable sensitivity, capable of detecting Fe(CN)63−/4− concentrations down to sub-picomolar levels. Utilising this ability to modulate redox reactions, we adapted the QMT probes to serve as electrochemical sensors for detecting viral proteins. By modifying the electrode surfaces, our functionalised QMT probes achieved sub-pM detection limits with high selectivity in biofluids such as nasopharyngeal secretions. These findings highlight the potential of QMT probes to develop into a new class of electrochemical tunnelling sensors, offering significant advancements in biomedical diagnostics.
Date Issued
2025-06-02
Date Acceptance
2025-02-17
Citation
Angewandte Chemie International Edition, 2025, 64 (23)
ISSN
1433-7851
Publisher
Wiley
Start Page
e202501941
Journal / Book Title
Angewandte Chemie International Edition
Volume
64
Issue
23
Copyright Statement
© 2025 Wiley-VCH GmbH. This is the author’s accepted manuscript made available under a CC-BY licence in accordance with Imperial’s Research Publications Open Access policy (www.imperial.ac.uk/oa-policy)
License URL
Identifier
https://www.ncbi.nlm.nih.gov/pubmed/39957485
Subjects
Quantum Tunnelling Sensors, Redox Cycling Reaction, Single-Molecular Detection, Confined Tunnelling Space, Biosensor
Publication Status
Published
Coverage Spatial
Germany
Article Number
e202501941
Date Publish Online
2025-03-04