Although plasmonic nanoparticles are widely utilized in spectroscopy and sensing applications, a quantitative
structure-function relationship is lacking. In this proceeding, we discuss measurements of single noble metal
nanoparticles using localized surface plasmon resonance (LSPR) spectroscopy, surface-enhanced Raman
spectroscopy (SERS), and transmission electron microscopy (TEM) to elucidate structure-function
relationships. A recently developed LSPR imaging spectroscopy instrument with an extremely fast camera
enables measurement of diffusion constants for individual silver nanoprisms dispersed in water-paving the
way for plasmonic particles as dynamic labels in biological systems. Correlated studies involving two or all
three of these techniques relate optical properties of the same nanoparticle to its structure. Lastly, single-molecule
surface-enhanced Raman spectroscopy of Rhodamine 6G is explored on lithographically fabricated
plasmonic structures.
In this work we perform correlated structural and optical studies of single nanoparticles as well as explore the generality
of SMSERS. First, wide-field plasmon resonance microscopy is used to simultaneously determine the LSPR spectra of
multiple Ag nanoprisms, whose structure is determined using TEM. Next, the structure-property relationships for well-defined
and easily-controlled nanoparticle structures (e.g. monomers, dimers, and trimers) are studied using correlated
TEM, LSPR, and SERS measurements of individual SERS nanotags. We present the SER spectrum of reporter
molecules on a single nanotag comprised of a Au trimer. It was determined that of 40 individual nanotags, just 19
exhibited SERS. The remaining nanoparticles were established by TEM to be monomers. These results demonstrate that
SERS signal is observed from individual nanotags containing a junction or hot spot. Lastly, we explore crystal violet, a
triphenyl methane dye that was used in the seminal SMSERS investigations, and re-examine single-molecule sensitivity
using the isotopologue approach.
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