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.