Silicon nanoclusters formed through self-assembly on CaF2 substrates: morphology and optical properties

Abstract

We studied the influence of the size and shape of silicon nanoclusters on their optical response. For this purpose, clusters were prepared by deposition, and subsequent diffusion and nucleation, of Si atoms on CaF2 substrate surfaces. By varying the growth parameters, oblate aggregates with sizes of between 5 and 30 nm and axial ratios between almost unity and 0.1 were generated. We found that the substrate temperature during growth predominantly influences the diameter and number density of the particles, whereas the coverage and deposition rate determine the axial ratio. Optical extinction was measured in the photon energy range between 1.0–6.0 eV and compared to model calculations. The mean size of the Si clusters mainly determines the absolute magnitude of the optical extinction. In contrast, the axial ratio drastically affects the overall structure of the spectra and the relative importance of three identified maxima. The most essential and interesting reason for the pronounced influence of the particle shape on the optical properties is a shift of the valence band plasmon in the silicon nanoparticles from an energy of above 9.0 eV for spherical clusters into the ultraviolet spectral range to about 5 eV for axial ratios below 0.3.