A Single-Step Bottom-up Approach for Synthesis of Highly Uniform Mie-Resonant Crystalline Semiconductor Particles at Visible Wavelengths.

Optically Mie-resonant crystalline silicon nanoparticles have long attracted interest for their unique scattering behaviors. Here, we report a bottom-up nonthermal plasma process that produces highly monodisperse particles, with diameters controllable between 60 and 214 nm, by temporarily electrostatically trapping nanoparticles inside a continuous-flow plasma reactor. The particle size is tuned by adjusting the gas residence time in the reactor. By dispersing the nanoparticles in water, optical extinction measurements indicate colloidal solutions of a particle-based metafluid in which particles support both strong magnetic and electric dipole resonances at visible wavelengths. The spectral overlap of the electric and magnetic resonances gives rise to directional Kerker scattering. The extinction measurements show excellent agreement with Mie theory, supporting the idea that the fabrication process enables particles with narrow distributions in size, shape, and composition. This single-step gas-phase process can also produce Mie-resonant nanoparticles of dielectric materials other than silicon and directly deposit them on the desired substrates.

Broadband, Angle- and Polarization-Invariant Antireflective and Absorbing Films by a Scalable Synthesis of Monodisperse Silicon Nanoparticles.

Optically induced magnetic resonances (OMRs) are highly tunable scattering states that cannot be reproduced in systems that only support electric resonances, such as in metals, lossy, or low-index materials. Despite offering unique scattering and coupling behavior, the study of OMRs in thin films has been limited by synthesis and simulation constraints. We report on the absorption and scattering response of OMR-based thin films composed of monodisperse crystalline silicon nanoparticles synthesized using a scalable nonthermal plasma growth technique and tractable simulation framework. The synthesis is solvent and ligand free, ensuring minimal contamination, and crystalline particles form with high yield and a narrow size distribution at close to room temperature. Using a scalable high-throughput deposition method, we deposit random particle films, without the need of a solid host matrix, showing near complete blackbody absorption at the collective OMR. This is achieved using 70% less material than an optimized antireflective-coated crystalline silicon thin film. The film exhibits strongly directional forward scattering with very low reflectivity, thus giving rise to angle- and polarization-insensitive antireflection properties across the visible spectrum. We find that, while commonly used effective medium models cannot capture the optical response, a modified effective medium accounting for multipole resonances and interparticle coupling shows excellent agreement with experiment. The effective permittivity and permeability are written in a mode and cluster resolved form, providing useful insight into how individual resonances and nanoparticle clusters affect the overall film response. Electric and magnetic-mode coupling show dramatically different behavior, resulting in uniquely different spectral broadening.

Design of efficient radiative emission and daytime cooling structures with Si3N4 and SiO2 nanoparticle laminate films.

Research on radiative cooling has attracted recent widespread interest owing to the potential for low-cost passive structures to enable large-scale thermal energy management. Using a generalized effective medium theory, we theoretically show that two-layer films comprised of SiO2 and Si3N4 nanoparticle layers on an Ag back reflector exhibit superior radiative cooling compared to single-layer or two-layer dense solid films, and can outperform other reported designs. The performance enhancement is a result of the ability to tune the nanoparticle fill fraction, which improves the spectral match between emissivity of this structure and the atmospheric transmission window. We also propose a standardized method for comparing the performance of radiative cooling structures reported by the research community.

Aluminum Oxide Nanoparticle Films Deposited from a Nonthermal Plasma: Synthesis, Characterization, and Crystallization.

Aluminum oxide, both in amorphous and crystalline forms, is a widely used inorganic ceramic material because of its chemical and structural properties. In this work, we synthesized amorphous aluminum oxide nanoparticles using a capacitively coupled nonthermal plasma utilizing trimethylaluminum and oxygen as precursors and studied their crystallization and phase transformation behavior through postsynthetic annealing. The use of two reactor geometries resulted in amorphous aluminum oxide nanoparticles with similar compositions but different sizes. Size tuning of these nanoparticles was achieved by varying the reactor pressure to produce amorphous aluminum oxide nanoparticles ranging from 6 to 22 nm. During postsynthetic annealing, powder samples of amorphous nanoparticles began to crystallize at 800 °C, forming crystalline θ and γ phase alumina. Their phase transformation behavior was found to be size-dependent in that powders of small 6 nm amorphous particles transformed to form phase-pure α-Al2O3 at 1100 °C, while powders of large 11 nm particles remained in the θ and γ phases. This phenomenon is attributed to the fast rate of densification and neck formation in small amorphous aluminum oxide particles.