Au nanoparticle monolayers: preparation, structural conversion and their surface-enhanced Raman scattering effects

An environment-friendly method is developed to fabricate close-packed Au nanoparticle (AuNP) monolayers with sub-10 nm interparticle spacing simply by covering n-butanol on the surface of an Au aqueous colloid. The close-packed nanostructure can further transform into two-dimensional (2D) aggregates with different aggregation degrees upon aging for several days. This structural evolution process was disclosed by transition electron microscopy (TEM) and UV-vis spectroscopy and its influence on the ensemble optical properties was further demonstrated by surface-enhanced Raman scattering (SERS). It was revealed that creating sub-10 nm interparticle spacing and particle dimers are highly desirable for engendering strong SERS activity under a 632.8 nm excitation. Further aging the film leads to the formation of larger aggregates, which moves the surface plasmon resonance of the aggregates gradually 'off-resonance' from the 632.8 nm excitation line and costs some numbers of sub-10 nm interparticle spacings. The two parameters together decrease the SERS activity of the close-packed AuNP monolayers. The present strategy thus provides an easy way to finely tune the SERS properties of thin nanoparticle films and other ensemble properties, which can easily be realized by creating sub-10 interparticle spacing, controlling the particle aggregation degree and by adopting suitable particle sizes and shapes.