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Enriching plasmon-enhanced Raman spectroscopy via electrochemistry and hybrid nanomaterials for trace chemical detection

Jones, Tabitha; (2024) Enriching plasmon-enhanced Raman spectroscopy via electrochemistry and hybrid nanomaterials for trace chemical detection. Doctoral thesis (Eng.D), UCL (University College London).

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Enriching plasmon-enhanced Raman spectroscopy via electrochemistry and hybrid nanomaterials for trace chemical detection - Tabitha Jones.pdf - Accepted Version
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Abstract

Biomarker detection is critical for effective disease diagnosis and treatment. Surface-enhanced Raman spectroscopy (SERS) has been heralded as a technique capable of achieving rapid, low-cost healthcare sensing. However, improvements are needed to enable quantitative detection in complex media, such as bodily fluids. This work explores ways to enrich SERS using electrochemistry, machine learning and hybrid nanomaterials. Two different approaches are developed in this thesis: an electrochemical SERS (E-SERS) system based on silver nanoparticle electrodes and a hybrid semiconductorplasmonic metal NP system. The E-SERS system was used to detect two important biomarkers, uric acid (UA) and creatinine (CRN). Applying an external potential enhances the SERS signal and enables multiplexed detection of the two analytes. Machine learning approaches were applied to a large E-SERS dataset (>2,300 spectra) to achieve quantitative, multiplexed detection of UA and CRN. Finally, proof-ofconcept experiments were performed in dilute synthetic urine to demonstrate the detection of clinically relevant concentrations of the analytes. A hybrid SERS system was fabricated using tin dioxide coated silver nanoparticles (Ag@SnO2 NPs). An unexpected, time-dependent increase in the SERS signal was observed when the Ag@SnO2 NP substrates were irradiated with the Raman laser. The in-situ laser enhancement enabled lower concentrations (<1 μM) of analytes to be detected compared to unirradiated substrates. Potential applications of the Ag@SnO2 NP system were demonstrated including the quantitative detection of uric acid, the indirect detection of the ketosis biomarker, 3-hydroxybutanoic acid, and the quantitative detection of ketamine in synthetic saliva.

Type: Thesis (Doctoral)
Qualification: Eng.D
Title: Enriching plasmon-enhanced Raman spectroscopy via electrochemistry and hybrid nanomaterials for trace chemical detection
Language: English
Additional information: Copyright © The Author 2024. Original content in this thesis is licensed under the terms of the Creative Commons Attribution-NonCommercial 4.0 International (CC BY-NC 4.0) Licence (https://creativecommons.org/licenses/by-nc/4.0/). Any third-party copyright material present remains the property of its respective owner(s) and is licensed under its existing terms. Access may initially be restricted at the author’s request.
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering
URI: https://discovery-pp.ucl.ac.uk/id/eprint/10194539
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