High-speed imaging of surface-enhanced Raman scattering fluctuations from individual nanoparticles

拉曼散射 纳米颗粒 材料科学 拉曼光谱 散射 纳米技术 曲面(拓扑) 光学 光电子学 物理 数学 几何学
作者
Nathan C. Lindquist,Carlos Diego L. de Albuquerque,Regivaldo G. Sobral-Filho,Irina Paci,Alexandre G. Brolo
出处
期刊:Nature Nanotechnology [Nature Portfolio]
卷期号:14 (10): 981-987 被引量:157
标识
DOI:10.1038/s41565-019-0535-6
摘要

The concept of plasmonic hotspots is central to the interpretation of the surface-enhanced Raman scattering (SERS) effect. Although plasmonic hotspots are generally portrayed as static features, single-molecule SERS (SM-SERS) is marked by characteristic time-dependent fluctuations in signal intensity. The origin of those fluctuations can be assigned to a variety of dynamic and complex processes, including molecular adsorption or desorption, surface diffusion, molecular reorientation and metal surface reconstruction. Since each of these mechanisms simultaneously contributes to a fluctuating SERS signal, probing their relative impact in SM-SERS remains an experimental challenge. Here, we introduce a super-resolution imaging technique with an acquisition rate of 800,000 frames per second to probe the spatial and temporal features of the SM-SERS fluctuations from single silver nanoshells. The technique has a spatial resolution of ~7 nm. The images reveal short ~10 µs scattering events localized in various regions on a single nanoparticle. Remarkably, even a fully functionalized nanoparticle was ‘dark’ more than 98% of the time. The sporadic SERS emission suggests a transient hotspot formation mechanism driven by a random reconstruction of the metallic surface, an effect that dominates over any plasmonic resonance of the particle itself. Our results provide the SERS community with a high-speed experimental approach to study the fast dynamic properties of SM-SERS hotspots in typical room-temperature experimental conditions, with possible implications in catalysis and sensing. An imaging technique can acquire surface-enhanced Raman scattering intensity fluctuations at 800,000 frames per second, revealing the dynamics of plasmonic hotspots at the single-particle level.
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