Novel optical devices such as biosensors, color displays and authentication devices can be obtained from the distinctive light scattering properties of resonant nanoparticles and nanostructured arrays. These arrays can be optimized through the choice of material, particle morphology and array geometry. In this thesis, by engineering the multi-frequency colorimetric responses of deterministic aperiodic nanostructured surfaces (DANS) with various spectral Fourier properties, I designed, fabricated and characterized scattering-based devices for optical biosensing and structural coloration applications.;In particular, using analytical and numerical optimization, colorimetric biosensors are designed and fabricated with conventional electron beam lithography, and characterized using dark-field scattering imaging as well as image autocorrelation analysis of scattered intensity in the visible spectral range. These sensors, which consist of aperiodic surfaces ranging from quasi-periodic to pseudo-random structures with flat Fourier spectra, sustain highly complex structural resonances that enable a novel optical sensing approach beyond the traditional Bragg scattering. To this end, I have experimentally demonstrated that DANS with engineered structural colors are capable of detecting nanoscale protein monolayers with significantly enhanced sensitivity over periodic structures. In addition, different aperiodic arrays of gold (Au) nanoparticles are integrated with polydimethylsiloxane (PDMS) microfluidic structures by soft-lithographic micro-imprint techniques. Distinctive scattering spectral shifts and spatial modifications of structural color patterns in response to refractive index variations were simultaneously measured. The successful integration of DANS with microfluidics technology has introduced a novel opto-fluidic sensing platform for label-free and multiplexed lab-on-a-chip applications.;Moreover, by studying the isotropic scattering properties of homogenized Pinwheel aperiodic arrays, angle-insensitive (i.e. isotropic) coloration from nanostructured metal surfaces can be designed and optimized without randomization. Pinwheel nanoparticle arrays on a gold thin film were fabricated for the first time and investigated using dark-field scattering and angle-resolved reflectivity measurements. In sharp contrast to the colorimetric responses of periodically nanopatterned surfaces, which strongly depend on the observation angle, spatially uniform and isotropic green coloration of gold films were demonstrated using these engineered metal surfaces. In addition, the intensity of the scattered light is enhanced by plasmonic resonance originated from gold nanoparticles deposited on the gold substrates. The development of the enhanced isotropic scattering devices could advance plasmonic applications to color display, optical tagging and colorimetric sensing technologies.
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