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

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.
Authors:
ORCiD logo [1] ;  [2] ; ORCiD logo [2] ;  [1] ; ORCiD logo [3] ;  [2] ;  [3] ;  [2] ; ORCiD logo [3] ; ORCiD logo [4] ; ORCiD logo [5] ; ORCiD logo [4]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). The Molecular Foundry; Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). The Molecular Foundry
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). The Molecular Foundry. Materials Sciences Division
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division; Univ. of Massachusetts, Amherst, MA (United States). Conte Center for Polymer Research. Polymer Science and Engineering Dept.; Beijing Univ. of Chemical Technology (China). Beijing Advanced Innovation Center for Soft Matter Science and Engineering; Tohoku Univ., Sendai (Japan). World Premier International Research Center Initiative–Advanced Inst. for Materials Research (WPI-AIMR)
Publication Date:
Grant/Contract Number:
AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
Journal Volume: 4; Journal Issue: 8; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1477357

Zhang, Ziyi, Jiang, Yufeng, Huang, Caili, Chai, Yu, Goldfine, Elise, Liu, Feng, Feng, Wenqian, Forth, Joe, Williams, Teresa E., Ashby, Paul D., Russell, Thomas P., and Helms, Brett A.. Guiding kinetic trajectories between jammed and unjammed states in 2D colloidal nanocrystal-polymer assemblies with zwitterionic ligands. United States: N. p., Web. doi:10.1126/sciadv.aap8045.
Zhang, Ziyi, Jiang, Yufeng, Huang, Caili, Chai, Yu, Goldfine, Elise, Liu, Feng, Feng, Wenqian, Forth, Joe, Williams, Teresa E., Ashby, Paul D., Russell, Thomas P., & Helms, Brett A.. Guiding kinetic trajectories between jammed and unjammed states in 2D colloidal nanocrystal-polymer assemblies with zwitterionic ligands. United States. doi:10.1126/sciadv.aap8045.
Zhang, Ziyi, Jiang, Yufeng, Huang, Caili, Chai, Yu, Goldfine, Elise, Liu, Feng, Feng, Wenqian, Forth, Joe, Williams, Teresa E., Ashby, Paul D., Russell, Thomas P., and Helms, Brett A.. 2018. "Guiding kinetic trajectories between jammed and unjammed states in 2D colloidal nanocrystal-polymer assemblies with zwitterionic ligands". United States. doi:10.1126/sciadv.aap8045. https://www.osti.gov/servlets/purl/1477357.
@article{osti_1477357,
title = {Guiding kinetic trajectories between jammed and unjammed states in 2D colloidal nanocrystal-polymer assemblies with zwitterionic ligands},
author = {Zhang, Ziyi and Jiang, Yufeng and Huang, Caili and Chai, Yu and Goldfine, Elise and Liu, Feng and Feng, Wenqian and Forth, Joe and Williams, Teresa E. and Ashby, Paul D. and Russell, Thomas P. and Helms, Brett A.},
abstractNote = {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.},
doi = {10.1126/sciadv.aap8045},
journal = {Science Advances},
number = 8,
volume = 4,
place = {United States},
year = {2018},
month = {8}
}

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