Plasmonic structures and their applications in nanoelectrochemistry and single-molecule spectroelectrochemistry

我们的研究项目集中在金属纳米结构的发展及其在表面增强现象、化学传感和光谱电化学（SEC）方面的应用。我们特别感兴趣的是在可见光范围内支持表面等离子体（SP）激发（局部或传播SPs）的纳米结构（等离子体结构）。最近，我们在等离子体动力学方面取得了以下重要突破，这些突破将最终推动单分子光谱电化学（SM-SEC）和纳米电化学的新方法的发展：1)我们观察到吸附在电极表面的染料的单分子表面增强拉曼散射（SM-SERS），并能够通过改变应用电位来控制单分子动力学；2)我们证明了金属薄膜上的纳米孔对吸附和支持增强光谱敏感。我们建议利用这些突破，进一步扩展SM-SEC在氧化还原系统和蛋白质吸附中的应用。我们还将使用“孔内”传感的概念来研究纳米孔内物质的电化学。纳米孔的光学性质将取决于被吸附分子的氧化态，这将是纳米孔结构中SEC的基础。此外，还将探讨使用形状纳米孔的表面增强SEC。

Our research program is centered on the development of metallic nanostructures and their applications in surface-enhanced phenomena, chemical sensing and spectroelectrochemistry (SEC). We are particularly interested in nanostructures that support surface plasmon (SP) excitations (either localized or propagating SPs) in the visible range (plasmonic structures). Recently, we have achieved the following important breakthroughs in plasmonics that will culminate in the development of new approaches for single-molecule spectroelectrochemistry (SM-SEC) and nanoelectrochemistry: 1) We observed single-molecule surface-enhanced Raman scattering (SM-SERS) from dyes adsorbed on an electrode surface and were able to control the single-molecule dynamics by changing the applied potential; 2) We demonstrated that nanoholes in metal films are sensitive to adsorption and support enhanced spectroscopy. We propose to capitalize on these breakthroughs by further extending the application of SM-SEC to redox systems and protein adsorption. We will also use the concept of "in-hole" sensing to study the electrochemistry of species inside the nanoholes. The optical properties of the nanoholes will depend on the oxidation state of the adsorbed molecules, which will be the basis for the SEC from the nanohole structures. Surface-enhanced SEC using shaped nanoholes will also be explored.