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Gelation of colloidal nanocrystals (NCs) emerged as a strategy to preserveinherent nanoscale properties in multiscale architectures. Yet availablegelation methods still struggle to reliably control nanoscale optical phenomenasuch as photoluminescence and localized surface plasmon resonance (LSPR) acrossNC systems due to processing variability. Here, we report on an alternativegelation method based on physical inter-NC interactions: short-rangedepletion-attractions balanced by long-range electrostatic repulsions. Thelatter are established by removing the native organic ligands that passivatetin-doped indium oxide (ITO) NCs while the former are introduced by mixing withsmall polyethylene glycol (PEG) chains. As we incorporate increasingconcentrations of PEG, we observe a reentrant phase behavior featuring twofavorable gelation windows; the first arises from bridging effects while thesecond is attributed to depletion-attractions according to phase behaviorpredicted by our unified theoretical model. The NCs remain discrete within thegel network, based on X-ray scattering and high-resolution transmissionelectron microscopy. The infrared optical response of the gel is reflective ofboth the NC building blocks and the network architecture, being characteristicof ITO NC LSPR with coupling interactions between neighboring NCs.

Gelation of Plasmonic Metal Oxide Nanocrystals by Polymer-Induced Depletion-Attractions