Abstract:
:Gelation of colloidal nanocrystals emerged as a strategy to preserve inherent nanoscale properties in multiscale architectures. However, available gelation methods to directly form self-supported nanocrystal networks struggle to reliably control nanoscale optical phenomena such as photoluminescence and localized surface plasmon resonance (LSPR) across nanocrystal systems due to processing variabilities. Here, we report on an alternative gelation method based on physical internanocrystal interactions: short-range depletion attractions balanced by long-range electrostatic repulsions. The latter are established by removing the native organic ligands that passivate tin-doped indium oxide (ITO) nanocrystals while the former are introduced by mixing with small PEG chains. As we incorporate increasing concentrations of PEG, we observe a reentrant phase behavior featuring two favorable gelation windows; the first arises from bridging effects while the second is attributed to depletion attractions according to phase behavior predicted by our unified theoretical model. Our assembled nanocrystals remain discrete within the gel network, based on X-ray scattering and high-resolution transmission electron microscopy. The infrared optical response of the gels is reflective of both the nanocrystal building blocks and the network architecture, being characteristic of ITO nanocrystals' LSPR with coupling interactions between neighboring nanocrystals.
journal_name
Proc Natl Acad Sci U S Aauthors
Saez Cabezas CA,Ong GK,Jadrich RB,Lindquist BA,Agrawal A,Truskett TM,Milliron DJdoi
10.1073/pnas.1806927115subject
Has Abstractpub_date
2018-09-04 00:00:00pages
8925-8930issue
36eissn
0027-8424issn
1091-6490pii
1806927115journal_volume
115pub_type
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