The progress in fundamental biological studies of disease has been revealing a variety of new biomarkers that are difficult to be detected by traditional diagnostic tools. Interestingly, plasmonics is an ultrasensitive optical technology applicable in medical diagnostics and biological imaging sensors. A dual-functional plasmonic substrate with a unique design that allows both the sensitive detection of photoluminescence (PL) via metal-enhanced photoluminescence (MEPL) and the specific Raman fingerprint via surface-enhanced Raman scattering (SERS) is highly desirable to improve accuracy and sensitivity in detection.
This dissertation describes the role of coupling agents, spacer effects, and importance characters of various platforms for the optimum bifunctional SERS-MEPL based on Ag@SiO2 core-shell nanocube(s) [NC(s)] for urinary biomarkers detection. In this work, the Ag NCs were synthesized by the polyol method and modified, firstly with different coupling agents, such as 3-mercaptopropyltrimethoxysilane (MPTMS) and 3-aminopropyltrimethoxysilane (APTMS), and secondly with tetraethylorthosilicate (TEOS). The presence of coupling agents greatly modified the Ag NC cores and manipulated the thickness and uniformity of the silica shells. Ultrathin silica-coated Ag NCs (with a ~1.5 nm silica layer) found to have a SERS intensity 3 fold higher than synthesized Ag NCs. In comparison with MPTMS, it was found that APTMS modified Ag@SiO2 NCs improved significant SERS and MEPL enhancements. Moreover, a ‘dual functionality’ represented by the simultaneous strengthening of SERS and MEPL signals can be achieved by mixing Ag@SiO2 NCs, with a silica shell thickness of ~1.5 nm and ~4.4 nm. This approach allows both the Ag@SiO2 NCs SERS and MEPL sensitivities to be maintained at ~90% after 12 weeks of storage.
Additionally, it is known that interactions between substrate and plasmonic nanostructures can influence the performance of plasmonic biosensing. Therefore, in the final approach, a substrate characterized with low refractive index and roughness was first fabricated by creating flower-like alumina on etched Al foil (f-Al2O3/e-Al). The Ag@SiO2 NCs assemble in the edge-edge configuration when they were deposited on this substrate. It is to note that the surface roughness of f-Al2O3/e-Al provides a pathway for the coupling of incident light to surface plasmon. The Ag@SiO2/f-Al2O3/e-Al substrate exhibits a coupling efficiency of laser light sources into surface plasmon hotspots for both SERS and MEPL. Moreover, the shelf life of this substrate is significantly improved due to reduced oxygen diffusion rate by ultrathin silica spacer and flower-like Al2O3 dielectric layer. Creatinine (CR) and flavin adenine dinucleotide (FAD) are biomolecules present in human blood and urine. With the advanced label-free SERS and MEPL techniques, these biomarkers in urine are detected, and it allows cheap, non-invasive and yet sensitive analysis.
The approaches explored in this dissertation could be developed as a powerful encoding tool for high-throughput bio-analysis.

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