Inhibiting Analyte Theft in Surface-Enhanced Raman Spectroscopy Substrates: Subnanomolar Quantitative Drug Detection.
de Nijs, Bart
American Chemical Society
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de Nijs, B., Carnegie, C., Szabó, I., Grys, D., Chikkaraddy, R., Kamp, M., Barrow, S. J., et al. (2019). Inhibiting Analyte Theft in Surface-Enhanced Raman Spectroscopy Substrates: Subnanomolar Quantitative Drug Detection.. ACS sensors, 4 (11), 2988-2996. https://doi.org/10.1021/acssensors.9b01484
Quantitative applications of surface enhanced Raman spectroscopy (SERS) often rely on surface partition layers grafted to SERS substrates to collect and trap solvated analytes that would not otherwise adsorb onto metals. Such binding layers drastically broaden the scope of analytes that can be probed. However, excess binding sites introduced by this partition layer also trap analytes outside the plasmonic ‘hot-spots’. We show that by eliminating these binding sites, limits of detection (LODs) can effectively be lowered by more than an order of magnitude. We highlight the effectiveness of this approach by demonstrating quantitative detection of controlled drugs down to sub-nanomolar concentrations in aqueous media. Such LODs are low enough to screen, for example, urine at clinically relevant levels. These findings provide unique insights into the binding behavior of analytes, which are essential when designing high performance SERS substrates.
In addition to the EPSRC funding B.d.N acknowledges support from the Leverhulme Trust and Isaac Newton Trust, C.C. acknowledges support from NPL (PO443073), R.C. acknowledges support from the Dr. Manmohan Singh scholarship from St. John’s College, M.K. thanks the European Commission for a Marie Skłodowska-Curie Fellowship (SPARCLEs, 7020005), S.J.B. thanks the European Commission for a Marie Skłodowska-Curie Fellowship (NANOSPHERE, 658360).
Isaac Newton Trust (18.08(K))
Leverhulme Trust (ECF-2018-021)
European Commission (658360)
EPSRC (via University of Exeter) (EP/R020965/1)
European Commission Horizon 2020 (H2020) Marie Sk?odowska-Curie actions (702005)
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External DOI: https://doi.org/10.1021/acssensors.9b01484
This record's URL: https://www.repository.cam.ac.uk/handle/1810/297437
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