Optical response of electro-tuneable 3D superstructures of plasmonic nanoparticles self-assembling on transparent columnar electrodes

Electrically tuneable, guided self-assembly of plasmonic nanoparticles (NPs) at polarized, patterned solid-liquid interfaces could enable numerous platforms for designing nanoplasmonic optical devices with new tuneable functionalities. Here, we propose a unique design of voltage-controlled guided 3D self-assembly of plasmonic NPs on transparent electrodes, patterned as columnar structures-arrays of vertical nanorods. NP assembly on the electrified surfaces of those columnar structures allows formation of a 3D superstructure of NPs, comprising stacking up of NPs in the voids between the columns, forming multiple NP-layers. A comprehensive theoretical model, based on quasi-static effective medium theory and multilayer Fresnel reflection scheme, is developed and verified against full-wave simulations for obtaining optical responses-reflectance, transmittance, and absorbance-from such systems of 3D self-assembled NPs. With a specific example of small gold nanospheres self-assembling on polarized zinc oxide columns, we show that the reflectance spectrum can be controlled by the number of stacked NP-layers. Numerical simulations show that peak reflectance can be enhanced up to ∼1.7 times, along with spectral broadening by a factor of ∼2-allowing wide-range tuning of optical reflectivity. Smaller NPs with superior mobility would be preferable over large NPs for realizing such devices for novel photonic and sensing applications.