High-Speed Fluctuation Analysis of Silver-Nanoparticle SERS in Solutions.

We analyzed the fluctuation of surface-enhanced Raman spectra with a temporal resolution of 25 ms using a conventional electron-multiplying charge-coupled device camera experimental setup. The signal-to-noise ratio of the spectra was improved using density-based spatial cluster analysis with noise. Silver nanoparticles (AgNPs) with different sizes were dispersed as surface-enhanced Raman spectroscopy platforms in violet aqueous solutions. The movement of AgNPs and the fluctuation of the spectra were characterized. The fluctuation (signal ON and OFF) was evaluated on the basis of the time intervals between ON and OFF timing. The behavior of each AgNP solution was explained by a two-dimensional random walk model, which means that the phenomenon was mainly governed by the Brownian motion of the AgNPs in the solution. The fluctuation was also compared among three different Raman modes, one of which showed anomalous behavior.