Designing optical metamaterials from colloidal nanocrystal assemblies
Cherie Kagan a
a University of Pennsylvania, 200 South 33rd Street, Philadelphia, 19104, United States
Proceedings of Internet NanoGe Conference on Nanocrystals (iNCNC)
Online, Spain, 2021 June 28th - July 2nd
Organizers: Maksym Kovalenko, Maria Ibáñez, Peter Reiss and Quinten Akkerman
Invited Speaker, Cherie Kagan, presentation 015
DOI: https://doi.org/10.29363/nanoge.incnc.2021.015
Publication date: 8th June 2021

Colloidal metallic and magnetic nanocrystals (NCs) are known for their size- and shape-dependent optical and magnetic properties and their solution-based printing and imprinting in device fabrication. We use NCs as building blocks of assemblies and exploit their chemical and physical (electrical, optical, magnetic, mechanical, thermal) tailorability to design and fabricate optical metamaterials. Chemical exchange of the long ligands used in NC synthesis with more compact ligand chemistries brings neighboring NCs into proximity, increasing interparticle coupling. For metal NCs, ligand-controlled coupling allows us to tune through a dielectric-to-metal phase transition, seen by a 1010 range in DC conductivity and a dielectric permittivity ranging from everywhere positive to everywhere negative across the whole range of optical frequencies [1], and is useful in the design of materials that are strong, ultrathin film optical absorbers [2] or strong optical scatterers [1], [3]. Addition of magnetic NCs, allows actuation of magnetic or mixed magnetic-metallic NC superstructures by external fields [4], [5]. Compact ligand exchange and thermal annealing of NC films also drives a large volume shrinkage in NC thin films, allowing a 10X tailorability in their Young’s modulus [5], [6]. By juxtaposing plasmonic NCs and bulk materials, we exploit their different chemical and mechanical properties to create misfit strain that drives the folding of NC/bulk bilayer heterostructures and the transformation of lithographically-defined two-dimensional structures into three-dimensional structures [5], [6]. We use the three-dimensional structures to demonstrate the scalable fabrication of large-area metamaterials with chiroptical responses of ~40% transmission difference between left-hand and right-hand circularly polarized light and that are suitable broadband circular polarizers [6], [7].

The authors are grateful for primary support of this work by the Office of Naval Research Multidisciplinary University Research
Initiative Award No. ONR N00014-18-1-2497.

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