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Title: Controlling Nanoparticle Orientations in the Self-Assembly of Patchy Quantum Dot-Gold Heterostructural Nanocrystals

Abstract

Self-assembly of nanocrystals is a promising route for creating macroscale materials that derive function from the properties of their nanoscale building blocks. While much progress has been made assembling nanocrystals into different superlattices, controlling the relative orientations of nanocrystals in those lattices remains a challenge. Here, we combine experiments with computer simulations to study the self-assembly of patchy heterostructural nanocrystals (HNCs), consisting of near-spherical quantum dots decorated with regular arrangements of small gold satellites, into close-packed superlattices with pronounced orientational alignment of HNCs. Our simulations indicate that the orientational alignment is caused by van der Waals interactions between gold patches and is sensitive to the interparticle distance in the superlattice. We demonstrate experimentally that the degree and type of orientational alignment can be controlled by changing ligand populations on HNCs. This study provides guidance for the design and fabrication of nanocrystal superlattices with enhanced structural control.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3];  [2];  [1];  [4];  [1];  [5]; ORCiD logo [6]; ORCiD logo [6]; ORCiD logo [6]; ORCiD logo [6];  [7]; ORCiD logo [8]; ORCiD logo [2]; ORCiD logo [1]
  1. Brown Univ., Providence, RI (United States)
  2. Univ. of Utah, Salt Lake City, UT (United States)
  3. Univ. of Florida, Gainesville, FL (United States)
  4. Max Planck Inst. for the Structure and Dynamics of Matter, Hamburg (Germany); Heinrich Petter Institute-Leibniz Inst. for Experimental Virology, Hamburg (Germany)
  5. Argonne National Lab. (ANL), Argonne, IL (United States)
  6. Univ. of Connecticut, Storrs, CT (United States)
  7. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
  8. Cornell Univ., Ithaca, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1524555
Report Number(s):
BNL-211720-2019-JAAM
Journal ID: ISSN 0002-7863
Grant/Contract Number:  
SC0012704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 141; Journal Issue: 14; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Zhu, Hua, Fan, Zhaochuan, Yu, Long, Wilson, Mitchell A., Nagaoka, Yasutaka, Eggert, Dennis, Cao, Can, Liu, Yuzi, Wei, Zichao, Wang, Xudong, He, Jie, Zhao, Jing, Li, Ruipeng, Wang, Zhongwu, Grünwald, Michael, and Chen, Ou. Controlling Nanoparticle Orientations in the Self-Assembly of Patchy Quantum Dot-Gold Heterostructural Nanocrystals. United States: N. p., 2019. Web. doi:10.1021/jacs.9b01033.
Zhu, Hua, Fan, Zhaochuan, Yu, Long, Wilson, Mitchell A., Nagaoka, Yasutaka, Eggert, Dennis, Cao, Can, Liu, Yuzi, Wei, Zichao, Wang, Xudong, He, Jie, Zhao, Jing, Li, Ruipeng, Wang, Zhongwu, Grünwald, Michael, & Chen, Ou. Controlling Nanoparticle Orientations in the Self-Assembly of Patchy Quantum Dot-Gold Heterostructural Nanocrystals. United States. doi:10.1021/jacs.9b01033.
Zhu, Hua, Fan, Zhaochuan, Yu, Long, Wilson, Mitchell A., Nagaoka, Yasutaka, Eggert, Dennis, Cao, Can, Liu, Yuzi, Wei, Zichao, Wang, Xudong, He, Jie, Zhao, Jing, Li, Ruipeng, Wang, Zhongwu, Grünwald, Michael, and Chen, Ou. Mon . "Controlling Nanoparticle Orientations in the Self-Assembly of Patchy Quantum Dot-Gold Heterostructural Nanocrystals". United States. doi:10.1021/jacs.9b01033. https://www.osti.gov/servlets/purl/1524555.
@article{osti_1524555,
title = {Controlling Nanoparticle Orientations in the Self-Assembly of Patchy Quantum Dot-Gold Heterostructural Nanocrystals},
author = {Zhu, Hua and Fan, Zhaochuan and Yu, Long and Wilson, Mitchell A. and Nagaoka, Yasutaka and Eggert, Dennis and Cao, Can and Liu, Yuzi and Wei, Zichao and Wang, Xudong and He, Jie and Zhao, Jing and Li, Ruipeng and Wang, Zhongwu and Grünwald, Michael and Chen, Ou},
abstractNote = {Self-assembly of nanocrystals is a promising route for creating macroscale materials that derive function from the properties of their nanoscale building blocks. While much progress has been made assembling nanocrystals into different superlattices, controlling the relative orientations of nanocrystals in those lattices remains a challenge. Here, we combine experiments with computer simulations to study the self-assembly of patchy heterostructural nanocrystals (HNCs), consisting of near-spherical quantum dots decorated with regular arrangements of small gold satellites, into close-packed superlattices with pronounced orientational alignment of HNCs. Our simulations indicate that the orientational alignment is caused by van der Waals interactions between gold patches and is sensitive to the interparticle distance in the superlattice. We demonstrate experimentally that the degree and type of orientational alignment can be controlled by changing ligand populations on HNCs. This study provides guidance for the design and fabrication of nanocrystal superlattices with enhanced structural control.},
doi = {10.1021/jacs.9b01033},
journal = {Journal of the American Chemical Society},
issn = {0002-7863},
number = 14,
volume = 141,
place = {United States},
year = {2019},
month = {3}
}

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Cited by: 11 works
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