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

Wray, Parker R. and Eslamisaray, Mohammad Ali and Nelson, Gunnar M. and Ilic, Ognjen and Kortshagen, Uwe R. and Atwater, Harry A. (2022) Broadband, Angle- and Polarization-Invariant Antireflective and Absorbing Films by a Scalable Synthesis of Monodisperse Silicon Nanoparticles. ACS Applied Materials & Interfaces, 14 (20). pp. 23624-23636. ISSN 1944-8244. doi:10.1021/acsami.2c03263. https://resolver.caltech.edu/CaltechAUTHORS:20220520-231858000

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Abstract

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.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/acsami.2c03263DOIArticle
ORCID:
AuthorORCID
Wray, Parker R.0000-0003-3384-0826
Eslamisaray, Mohammad Ali0000-0001-8704-592X
Kortshagen, Uwe R.0000-0001-5944-3656
Atwater, Harry A.0000-0001-9435-0201
Additional Information:© 2022 American Chemical Society. Received: February 21, 2022; Accepted: April 15, 2022; Published: May 12, 2022. This work is supported by the Army Research Office under MURI project under W911NF-18-1-0240. Portions of this work were conducted in the Minnesota Nano Center, which is supported by the National Science Foundation through the National Nanotechnology Coordinated Infrastructure (NNCI) under Award Number ECCS-2025124. O.I. also acknowledges support from the 3M Foundation through the 3M Non-Tenured Faculty Award grant. Author Contributions. P.R.W. and M.A.E. contributed equally. P.R.W. conceived the idea, designed the experiments, developed the effective medium theory, and performed calculations, analysis, and interpretation of results pertaining to the electromagnetic aspects of the project. M.A.E. designed the nonthermal plasma reactor for nanoparticle synthesis and film deposition, and performed TEM for characterization of particle size, shape, and crystallinity. G.M.N. performed optical measurements of the particle film with oversight by P.R.W. and, with help from M.A.E., performed SEM and density calculations to determine the particle film’s fill fraction and structure. H.A.A., U.R.K., and O.I. oversaw the project. All authors contributed to writing and editing the manuscript. The authors declare no competing financial interest.
Funders:
Funding AgencyGrant Number
Army Research Office (ARO)W911NF-18-1-0240
NSFECCS-2025124
3M FoundationUNSPECIFIED
Subject Keywords:antireflection; absorber nanoparticles; nanocrystals; optical magnetic resonance; plasma films
Issue or Number:20
DOI:10.1021/acsami.2c03263
Record Number:CaltechAUTHORS:20220520-231858000
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20220520-231858000
Official Citation:Broadband, Angle- and Polarization-Invariant Antireflective and Absorbing Films by a Scalable Synthesis of Monodisperse Silicon Nanoparticles. Parker R. Wray, Mohammad Ali Eslamisaray, Gunnar M. Nelson, Ognjen Ilic, Uwe R. Kortshagen, and Harry A. Atwater. ACS Applied Materials & Interfaces 2022 14 (20), 23624-23636; DOI: 10.1021/acsami.2c03263
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:114869
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:24 May 2022 14:36
Last Modified:08 Jun 2022 16:42

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