Summary: | Here, highly transparent nanocomposite films with an adjustable refractive index were fabricated through stable dispersion of ZrO<sub>2</sub> (<i>n</i> = 2.16) nanoparticles (NPs) subjected to surface modification with SiO<sub>2</sub> (<i>n</i> = 1.46) in polydimethylsiloxane (PDMS) (<i>n</i> = 1.42) using the Stöber method. ZrO<sub>2</sub> NPs (13.7 nm) were synthesized using conventional hydrothermal synthesis, and their surface modification with SiO<sub>2</sub> (ZrO<sub>2</sub>@SiO<sub>2</sub> NPs) was controlled by varying the reaction time (3–54 h). The surface modification of the NPs was characterized using Fourier-transform infrared spectroscopy, dynamic light scattering, X-ray photoelectron spectroscopy, scanning electron microscopy, transmission electron microscopy, and ellipsometry. The surface modification was monitored, and the effective layer thickness of SiO<sub>2</sub> varied from 0.1 nm to 4.2 nm. The effective refractive index of the ZrO<sub>2</sub>@SiO<sub>2</sub> NPs at λ = 633 nm was gradually reduced from 2.16 to 1.63. The 100 nm nanocomposite film was prepared by spin-coating the dispersion of ZrO<sub>2</sub>@SiO<sub>2</sub> NPs in PDMS on the coverslip. The nanocomposite film prepared using ZrO<sub>2</sub>@SiO<sub>2</sub> NPs with a reaction time of 18 h (ZrO<sub>2</sub>@SiO<sub>2</sub>-18h-PDMS) exhibited excellent optical transparency (T<sub>average</sub> = 91.1%), close to the transparency of the coverslip (T<sub>average</sub> = 91.4%) in the visible range, and an adjustable refractive index (<i>n</i> = 1.42–1.60) as the NP content in the film increased from 0 to 50.0 wt%.
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