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Sci Adv. 2018 Aug 3;4(8):eaap8045. doi: 10.1126/sciadv.aap8045. eCollection 2018 Aug.

Guiding kinetic trajectories between jammed and unjammed states in 2D colloidal nanocrystal-polymer assemblies with zwitterionic ligands.

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The Molecular Foundry, Lawrence Berkeley National Laboratory, One Cyclotron Road, Berkeley, CA 94720, USA.
Department of Materials Science and Engineering, University of California, Berkeley, Hearst Mining Building, Berkeley, CA 94720, USA.
Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.
Polymer Science and Engineering Department, University of Massachusetts, 120 Governors Drive, Conte Center for Polymer Research, Amherst, MA 01003, USA.
Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China.
World Premier International Research Center Initiative-Advanced Institute for Materials Research (WPI-AIMR), Tohoku University, 2-1-1 Katahira, Aoba, Sendai 980-8577, Japan.


Mesostructured matter composed of colloidal nanocrystals in solidified architectures abounds with broadly tunable catalytic, magnetic, optoelectronic, and energy storing properties. Less common are liquid-like assemblies of colloidal nanocrystals in a condensed phase, which may have different energy transduction behaviors owing to their dynamic character. Limiting investigations into dynamic colloidal nanocrystal architectures is the lack of schemes to control or redirect the tendency of the system to solidify. We show how to solidify and subsequently reconfigure colloidal nanocrystal assemblies dimensionally confined to a liquid-liquid interface. Our success in this regard hinged on the development of competitive chemistries anchoring or releasing the nanocrystals to or from the interface. With these chemistries, it was possible to control the kinetic trajectory between quasi-two-dimensional jammed (solid-like) and unjammed (liquid-like) states. In future schemes, it may be possible to leverage this control to direct the formation or destruction of explicit physical pathways for energy carriers to migrate in the system in response to an external field.

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