Aggregation of Silica Nanoparticles in Sol–Gel Processes to Create Optical Coatings with Controllable Ultralow Refractive Indices

Optical coatings with controllable ultralow refractive indices are of profound significance in optical areas. However, it remains a challenge to fabricate such coatings using a simple method. Here we develop an effective and simple approach to create ultra-low-index coatings. This approach was based on a modified sol-gel process, with a key process that involved the aggregation of silica nanoparticles via the addition of a polymer surfactant (e.g., polyvinylpyrrolydone) in sols before coating. The approach involves three steps: the synthesis of silica sols under ammonia catalysis in ethanol (Stöber method), the addition of polyvinylpyrrolydone in the silica sols to induce the aggregation of the silica nanoparticles, and the formation of ultra-low-index coatings by depositing the aggregated silica sols on substrates. Through varying the aggregation extent, this approach produced coatings with controllable refractive indices ranging from 1.17 to 1.07. To the best of our knowledge, the minimum index value of 1.07 from our coating is among the lowest refractive indices ever reported. The ultra-low-index coatings demonstrated excellent optical properties, with which perfect quarter-wavelength antireflection coatings (maximum transmittance ∼100%) and broadband antireflection coatings (transmittance >98% from 400 to 1100 nm) can be prepared. One advantage of the antireflection coatings is that their transmission is less dependent on the refractive index and the thickness of the stacking layer, which make it promising in large-scale production. Moreover, the coatings can be made hydrophobic (water contact angle 136°) by exposing the coatings to a hexamethyldisilazane atmosphere, exhibiting high environmental stability in a humid environment. The aggregation of silica nanoparticles in sol-gel processes provides a scalable alternative to the current approaches for creating ultra-low-index coatings.