Metasurfaces are nanophotonic elements that allow for the controlled manipulation of light. Many applications require control of both the angular and spectral responses of a single metasurface, for example, in light trapping for thin-film photovoltaic absorbers. Existing design approaches often rely on iterative optimization and do not provide interpretable handles at the design stage for controlling angle and spectral responses.

This thesis introduces and validates a design framework for correlated-disordered metasurfaces that provides design-stage control over angular and spectral scattering responses. The underlying correlated-disordered point lattice is obtained by prescribing spatial correlations directly in Fourier space and discretizing the real space into a set of coordinates. The prescribed spatial correlations are preserved in the discretization and determine the angular scattering response of the ensemble. The lattice is decorated with nanoscatterers, whose geometries determine each nanoscatterer's resonant response and thereby modulate the metasurface's spectral response. Angular scattering control is experimentally validated using Fourier scatterometry, while spectral behavior is computationally assessed.

The framework is extended to the interleaving of two independently designed correlated-disordered metasurfaces into a single plane. The combined angular scattering response is approximately additive, as shown experimentally. Computational results indicate a similar preservation of the spectral scattering response, revealing that the individual scattering behavior is largely preserved during the interleaving step, with observable cross-talk between the two metasurfaces. A systematic computational study further investigates how variations in the key design parameters within this framework influence the collective scattering response.

Light trapping in thin-film photovoltaic absorbers is an established problem in nanophotonics, where angular and spectral control of incident light can improve performance by coupling it to guided-mode resonances. The design framework enables the realization of multi-resonant, correlated-disordered light-trapping patterns by interleaving two metasurfaces with distinct spatial correlations and resonator geometries, thereby combining prescribed angular redistribution with discrete multi-resonant elements. Compared with double-periodic patterns with the same two resonator geometries and with interconnected correlated-disordered patterns that share similar structural correlations but lack discrete resonators, this approach yields higher absorption in a thin-film absorber, as revealed by computational investigation.

Zinc phosphide is chosen as a demonstrator material in this thesis. The stability of this emerging photovoltaic material, made from earth-abundant elements, under atmospheric conditions is investigated. A long-term experimental study identifies surface oxidation as the dominant degradation mechanism, which can be mitigated by a thin dielectric capping layer.

Together, these results establish a non-iterative and interpretable design methodology for correlated-disordered metasurfaces by combining the reciprocal-space prescription with discrete resonator decoration and interleaving strategies. Demonstrated for thin-film light trapping, the approach generalizes to metasurface design problems that benefit from the joint engineering of spatial correlations and resonant building blocks.