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Surface enhanced Raman spectroscopy (SERS) was used to probe the surfacechemistry of chlorine-terminated silicon nanocrystal (Si-NC) surfaces in anair-free environment. SERS effect was observed from the thin films of Ag$_x$Ousing 514 nm laser wavelength. When a monolayer of Si-NCs were spin-coated onAg$_x$O SERS substrates, a very clear signal of surface states, includingSi-Cl$_x$, and Si-H$_x$ were observed. Upon air-exposure, we observed thetemporal reduction of Si-Cl$_x$ peak intensity, and a development ofoxidation-related peak intensities, like Si-O$_x$ and Si-O-H$_x$. In addition,first, second and third order transverse optical (TO) modes of Si-NCs were alsoobserved at 519, 1000 and 1600 cm$^{-1}$, respectively. As a comparison, Ramananalysis of a thick film (> 200 nm) of Si-NCs deposited on ordinary glasssubstrates were performed. This analysis only demonstrated the first TO mode ofSi-NCs, and the all the other features originated from SERS enhancement did notappear in the spectrum. These results conclude that, SERS is not only capableof single-molecule detection, but also a powerful technique for monitoring thesurface chemistry of nanoparticles.

Chemical analysis of ligand-free silicon nanocrystal surfaces by surface enhanced Raman spectroscopy