Year: 2018
Type: dissertation
Abstract: The world’s booming population projected to reach 10 billion by 2050 causes enormous stresses on environmental safety, food supply, and healthcare, which in return threatens human civilizations. One of the most promising solutions lies at innovating point-of-care (POC) sensing technologies to conduct detection of environmental hazards, monitoring of food safety, and early diagnosis of diseases in a timely and accurate manner. The discovery of surface-enhanced spectroscopy in the 1970s has significantly stimulated research on light-matter interaction which gives rise to enhanced optical phenomena such as surface-enhanced Raman scattering (SERS), plasmon-enhanced fluorescence (PEF), and particularly, they have found enormous applications in optical sensing. To fully exploit surface-enhanced spectroscopy to advance sensing technologies, it requires innovations in the sensor design as well as the plasmonic metallic nanostructures, which is exactly the focus of this dissertation. Owing to their strong capabilities of revealing molecular fingerprints and conducting single molecule analysis, both SERS and PEF have received extensive research interests. Since SERS directly correlates with the local electromagnetic (EM) field enhancement, it is featured by the simplicity in signal amplification. However, high SERS spectral resolution cannot be achieved without a tightly focused laser beam, which compromises the design of SERS-based POC sensing platforms. In contrast, the emission nature of fluorescence makes PEF easily coupled with POC readers, but optimal PEF requires a delicate control of the separation distance between the fluorophore and the nanostructure to minimize fluorescence quenching. SERS and PEF are essentially two complementary techniques and both hold great promise for POC sensing technologies. In the dissertation, in the first place, two label-free SERS sensors have been developed aiming to reduce the number of elements used in a sensor, which could potentially minimize interference, reduce the cost, and enhance the performance. In this regard, a label-free SERS sensor for mercury ions (Hg2+) detection has been developed based on functionalized gold nanoparticles, which employs a small molecule 4-mercaptobenzoic acid to capture mercury ions. A coordination bond formed only in the presence of mercury ions produces a new SERS peak at 374 cm-1, allowing unique detection of mercury ions. The other label-free SERS sensor has been developed for nitrite (NO2-) detection following the mechanism of Griess reaction based on the plasmonic coupling between gold nanostars and silver nanopyramid arrays. A newly formed azo compound produces at least three characteristic SERS peaks at 1140 cm-1, 1389 cm-1, and 1434 cm-1, which allow a highly specific detection
DOI: 10.33915/etd.3710
Author: Peng Zheng
Institution: West Virginia University
Language: English
Field: Materials Science
Domain: Physical Sciences
Open Access status: gold
OpenAlex ID: W2906488285