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Nanoparticle aggregate structures allow for efficient photon capture, and thus exhibit excellent optical absorption properties. In this study, a model of randomly distributed nanochain aggregates on silicon substrates is developed and analyzed. The Gaussian, uniform, and Cauchy spatial distribution functions are used to characterize the aggregate forms of the nanochains and their morphologies are realistically reconstructed. The relationships between the structural parameters (thickness and filling factor), equivalent physical parameters (density, heat capacity, and thermal conductivity), and visible absorptivity of the structures are established and analyzed. All the above-mentioned parameters exhibit extreme values, which maximize the visible-range absorption; these values are determined by the material properties and nanochain aggregate structure. Finally, Al nanochain aggregate samples are fabricated on Si substrates by reducing the kinetic energy of the metal vapor during deposition. The spectral reflection characteristics of the samples are studied experimentally. The Spearman correlation coefficients for the calculated spectral absorption curves and those measured experimentally are higher than 0.82, thus confirming that the model is accurate. The relative errors between the calculated visible-range absorptivities and the measured data are less than 0.3%, further confirming the accuracy of the model.

We demonstrate a concept and fabrication of lithography-free layered metal-SiO2 thin-film structures which have reduced reflectivity (black appearance), to as low as 0.9%, with 4.9% broadband reflectance (8.9% for soda lime) in the 500-1400 nm range. The multi-layered (four layers) thin-film metamaterial is designed so that optical impedance matching produces minimal reflectance and transmittance within the visible and infra-red (IR) spectral region for a range of incident angles. The structure has enhanced absorbance and is easily tuned for reduced minimal transmission and reflection. This approach should allow for novel anti-reflection surfaces by impedance matching to be realized.

We program the optical properties of colloidal Au nanocrystal (NC) assemblies via an unconventional ligand hybridization (LH) strategy to precisely engineer interparticle interactions and design materials with optical properties difficult or impossible to achieve in bulk form. Long-chain hydrocarbon ligands used in NC synthesis are partially exchanged, from 0% to 100%, with compact thiocyanate ligands by controlling the reaction time for exchange. The resulting NC assemblies show transmittance, reflectance, optical permittivity, and direct-current (DC) resistivity that continuously traverse a dielectric-metal transition, providing analog tuning of their physical properties, unlike the digital control realized by complete exchange with ligands of varying length. Exploiting this LH strategy, we create Au NC assemblies that are strong, ultrathin film optical absorbers, as seen by a 6× increase in the extinction of infrared light compared to that in bulk Au thin films and by a temperature rise of 20 °C upon illumination with 808 nm light. Our LH strategy may be applied to the design of materials constructed from NCs of different size, shape, and composition for specific applications.