Engineering Chromatic Intensity Through Sol–Gel Confinement in Melanin–Silica Hybrids

Melanin is a biological pigment known for its broadband UV-Vis absorption and structural disorder, which collectively determine its chromatic response. In this study, melanin–silica hybrid materials were synthesized via sol–gel processing under different catalytic conditions (acid, base, sequential acid–base) and using distinct silica precursors (TEOS and sodium metasilicate) to investigate how the inorganic matrix modulates the optical properties of the synthetic melanin. Colorimetric analysis revealed significant variations in lightness among the hybrids, while the chromatic coordinates remained characteristic of eumelanin. The material obtained via the sequential acid–base route exhibited the lowest lightness and highest absorption, indicating more efficient pigment dispersion, whereas the system derived from silicate precursors showed the highest lightness and lowest absorption, suggesting increased light scattering and/or pigment aggregation. Materials prepared under purely acidic and basic conditions displayed intermediate optical behavior. Electron Microscopy revealed distinct morphologies associated with each synthesis pathway, ranging from dense lamellar structures to compact aggregates and hierarchical assemblies, directly influencing light scattering mechanisms. Thermal analysis confirmed effective stabilization of melanin within the silica networks, with significantly reduced mass loss compared to the pure pigment. Confocal microscopy revealed detectable fluorescence only in selected systems, indicating variations in pigment dispersion and aggregation state. Overall, the results demonstrate that the chromatic response of melanin–silica hybrids is governed not only by the intrinsic properties of the pigment, but also by the structural organization of the inorganic matrix. Sol–gel processing thus provides a versatile strategy for tuning the optical behavior of melanin-based materials through controlled interfacial interactions.