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Films of close-packed Au nanoparticles are coupled electrodynamically throughtheir collective plasmon resonances. This collective optical response resultsin enhanced light-matter interactions, which can be exploited in variousapplications. Here, we demonstrate their application in sensing volatileorganic compounds, using methanol as a test-case. Ordered films over severalcm2 were obtained by interfacial self-assembly of colloidal Au nanoparticles(~10 nm diameter) through controlled evaporation of the solvent. Even thoughisolated nanoparticles of this size are inherently non-scattering, whenarranged in a close-packed film the plasmonic coupling results in a strongreflectance and absorbance. The in-situ tracking of vapor phase methanolconcentration through UV-Vis transmission measurements of the nanoparticle filmis first demonstrated. Next, in-situ ellipsometry of the self-assembled filmsin the Kretschmann (also known as ATR) configuration is shown to yield enhancedsensitivity, especially with phase difference measurements. Our study shows theexcellent agreement between theoretical models of the spectral response ofself-assembled films with experimental in-situ sensing experiments. At the sametime, the theoretical framework provides the basis for the interpretation ofthe various observed experimental trends. Combining periodic nanoparticle filmswith ellipsometry in the Kretschmann configuration is a promising strategytowards highly sensitive and selective plasmonic thin-film devices based oncolloidal fabrication methods for volatile organic compound (VOC) sensingapplications.

Self-Assembled Ligand-Capped Plasmonic Au Nanoparticle Films in the Kretschmann Configuration for Sensing of Volatile Organic Compounds