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Title: Biomimetic Hierarchical Assembly of Helical Supraparticles from Chiral Nanoparticles

Chiroptical materials found in butterflies, beetles, stomatopod crustaceans, and other creatures are attributed to biocomposites with helical motifs and multiscale hierarchical organization. These structurally sophisticated materials self-assemble from primitive nanoscale building blocks, a process that is simpler and more energy efficient than many top-down methods currently used to produce similarly sized three-dimensional materials. In this paper, we report that molecular-scale chirality of a CdTe nanoparticle surface can be translated to nanoscale helical assemblies, leading to chiroptical activity in the visible electromagnetic range. Chiral CdTe nanoparticles coated with cysteine self-organize around Te cores to produce helical supraparticles. D-/L-Form of the amino acid determines the dominant left/right helicity of the supraparticles. Coarse-grained molecular dynamics simulations with a helical pair-potential confirm the assembly mechanism and the origin of its enantioselectivity, providing a framework for engineering three-dimensional chiral materials by self-assembly. Finally, the helical supraparticles further self-organize into lamellar crystals with liquid crystalline order, demonstrating the possibility of hierarchical organization and with multiple structural motifs and length scales determined by molecular-scale asymmetry of nanoparticle interactions.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [4] ;  [5] ;  [6] ;  [7] ;  [8] ;  [9]
  1. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Chemical Engineering; Wenzhou Medical Univ. (China). Wenzhou Inst. of Biomaterials and Engineering
  2. Univ. of Michigan, Ann Arbor, MI (United States). Biointerfaces Inst. Dept. of Materials Science and Engineering
  3. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Chemical Engineering. Biointerfaces Inst.
  4. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Chemical Engineering
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Center for Electron Microscopy. Molecular Foundry
  6. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Materials Science and Engineering
  7. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Chemical Engineering; Myongji Univ., Yongin (Korea, Republic of). Dept. of Chemical Engineering
  8. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Chemical Engineering. Biointerfaces Inst. Dept. of Materials Science and Engineering
  9. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Chemical Engineering. Biointerfaces Inst. Dept. of Materials Science and Engineering. Dept. of Biomedical Engineering
Publication Date:
Grant/Contract Number:
AC02-05CH11231; DMR 1120923; DMR-0320740; DMR-9871177; ECS-0601345; CBET 0933384; CBET 0932823; CBET 1036672; ARO MURI W911NF-10-1-0518; NSFC-21573162; WIBEZD2014001-02
Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 10; Journal Issue: 3; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of Michigan, Ann Arbor, MI (United States); Wenzhou Medical Univ. (China)
Sponsoring Org:
USDOE Office of Science (SC); National Science Foundation (NSF); US Army Research Office (ARO); National Natural Science Foundation of China (NNSFC)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; biomimetic nanoparticles; chirality; helices; self-assembly; supraparticles; virus-like nanostructures
OSTI Identifier:
1440921

Zhou, Yunlong, Marson, Ryan L., van Anders, Greg, Zhu, Jian, Ma, Guanxiang, Ercius, Peter, Sun, Kai, Yeom, Bongjun, Glotzer, Sharon C., and Kotov, Nicholas A.. Biomimetic Hierarchical Assembly of Helical Supraparticles from Chiral Nanoparticles. United States: N. p., Web. doi:10.1021/acsnano.5b05983.
Zhou, Yunlong, Marson, Ryan L., van Anders, Greg, Zhu, Jian, Ma, Guanxiang, Ercius, Peter, Sun, Kai, Yeom, Bongjun, Glotzer, Sharon C., & Kotov, Nicholas A.. Biomimetic Hierarchical Assembly of Helical Supraparticles from Chiral Nanoparticles. United States. doi:10.1021/acsnano.5b05983.
Zhou, Yunlong, Marson, Ryan L., van Anders, Greg, Zhu, Jian, Ma, Guanxiang, Ercius, Peter, Sun, Kai, Yeom, Bongjun, Glotzer, Sharon C., and Kotov, Nicholas A.. 2016. "Biomimetic Hierarchical Assembly of Helical Supraparticles from Chiral Nanoparticles". United States. doi:10.1021/acsnano.5b05983. https://www.osti.gov/servlets/purl/1440921.
@article{osti_1440921,
title = {Biomimetic Hierarchical Assembly of Helical Supraparticles from Chiral Nanoparticles},
author = {Zhou, Yunlong and Marson, Ryan L. and van Anders, Greg and Zhu, Jian and Ma, Guanxiang and Ercius, Peter and Sun, Kai and Yeom, Bongjun and Glotzer, Sharon C. and Kotov, Nicholas A.},
abstractNote = {Chiroptical materials found in butterflies, beetles, stomatopod crustaceans, and other creatures are attributed to biocomposites with helical motifs and multiscale hierarchical organization. These structurally sophisticated materials self-assemble from primitive nanoscale building blocks, a process that is simpler and more energy efficient than many top-down methods currently used to produce similarly sized three-dimensional materials. In this paper, we report that molecular-scale chirality of a CdTe nanoparticle surface can be translated to nanoscale helical assemblies, leading to chiroptical activity in the visible electromagnetic range. Chiral CdTe nanoparticles coated with cysteine self-organize around Te cores to produce helical supraparticles. D-/L-Form of the amino acid determines the dominant left/right helicity of the supraparticles. Coarse-grained molecular dynamics simulations with a helical pair-potential confirm the assembly mechanism and the origin of its enantioselectivity, providing a framework for engineering three-dimensional chiral materials by self-assembly. Finally, the helical supraparticles further self-organize into lamellar crystals with liquid crystalline order, demonstrating the possibility of hierarchical organization and with multiple structural motifs and length scales determined by molecular-scale asymmetry of nanoparticle interactions.},
doi = {10.1021/acsnano.5b05983},
journal = {ACS Nano},
number = 3,
volume = 10,
place = {United States},
year = {2016},
month = {2}
}