The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adom.201900428. Structural ColorationThe natural world provides a vast number of inspirational sources for the design and development of new materials with outstanding properties. The feather barbs of the plum-throated cotinga is one out of many examples for demonstrating the way by which nature generates intense colors based on the mechanism of structural coloration and without the need for pigments. [1,2] Structural colors are the result of spectrally selective light scattering caused by nanostructures whereas the color

Angle independent non-absorbing spectral filters are required for many applications such as sunscreens, structural colors, photovoltaics, and radiative cooling. One of the promising and simple to manufacture structures is based on the disordered arrangement of monodisperse spherical particles by self-assembly, also called photonic glasses. So far, reported photonic glasses inherently show poor spectral selectivity with a smooth transition in reflection. No significant improvement is usually expected from particles optimization as the Mie resonances are broad for small dielectric particles with a moderate refractive index. Via Fourier space engineering, we show here that it is, nonetheless, possible to obtain sharp spectral transitions from the synergetic effect of a core-shell geometry of the particles with the short range order of the photonic glass. We apply the developed approach to demonstrate a high color saturation of a non-iridescent blue structural color employing a photonic glass with hollow sphere particles, which features a sharp spectral transition in reflection. The experimental results support the theoretical predictions from the first-order approximation.

To obtain high-quality homogeneous photonic glass-based structural color films over large areas, it is essential to precisely control the degree of disorder of the spherical particles used and reduce the crack density within the films as much as possible. To tailor the disorder and quality of photonic glasses, a heteroaggregation-based process was developed by employing two oppositely charged equal-sized polystyrene (PS) particle types. The influence of the particle size ratio on the extent of heteroaggregation in the suspension mixes is investigated and correlated with both the morphology and the resultant optical properties of the films. The results show that the oppositely charged particle size ratio within the mix greatly influences the assembled structure in the films, affecting their roughness, crack density, and the coffee-ring formation. To better differentiate the morphology of the films, scanning electron microscopy images of the microstructures were classified by a supervised training of a deep convolutional neural network model to find distinctions that are inaccessible by conventional image analysis methods. Selected compositions were then infiltrated with TiO2 via atomic layer deposition, and after removal of the PS spheres, surface-templated inverse photonic glasses were obtained. Different color impressions and optical properties were obtained depending on the heteroaggregation level and thus the quality of the resultant films. The best results regarding the stability of the films and suppression of coffee-ring formation are obtained with a 35 wt % positively charged over negatively charged particle mix, which yielded enhanced structural coloration associated with improved film quality, tailored by the heteroaggregation fabrication process.

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