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Title: Self-Assembly of Quantum Dot–Gold Heterodimer Nanocrystals with Orientational Order

Abstract

The self-assembly of nanocrystals into ordered superlattices is a powerful strategy for the production of functional nanomaterials. The assembly of well-ordered target structures, however, requires control over the building blocks’ size and shape as well as their interactions. While nanocrystals with homogeneous composition are now routinely synthesized with high precision and assembled into various ordered structures, high-quality multicomponent nanocrystals and their ordered assemblies are rarely reported. In this paper, we demonstrate the synthesis of quantum dot–gold (QD-Au) heterodimers. These heterodimers possess a uniform shape and narrow size distribution and are capped with oleylamine and dodecyltrimethylammonium bromide (DTAB). Assembly of the heterodimers results in a superlattice with long-range orientational alignment of dimers. Using synchrotron-based X-ray measurements, we characterize the complex superstructure formed from the dimers. Molecular dynamics simulations of a coarse-grained model suggest that anisotropic interactions between the quantum dot and gold components of the dimer drive superlattice formation. The high degree of orientational order demonstrated in this work is a potential route to nanomaterials with useful optoelectronic properties.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [1];  [2];  [1];  [3]; ORCiD logo [3];  [4]; ORCiD logo [2]; ORCiD logo [1]
  1. Brown Univ., Providence, RI (United States). Dept. of Chemistry
  2. Univ. of Utah, Salt Lake City, UT (United States). Dept. of Chemistry
  3. Univ. of Connecticut, Storrs, CT (United States). Dept. of Chemistry
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1475146
Report Number(s):
BNL-209103-2018-JAAM
Journal ID: ISSN 1530-6984
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 18; Journal Issue: 8; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Self-assembly; colloidal nanocrystals; heterodimer; anisotropic interparticle interactions; molecular dynamics simulation

Citation Formats

Zhu, Hua, Fan, Zhaochuan, Yuan, Yucheng, Wilson, Mitchell A., Hills-Kimball, Katie, Wei, Zichao, He, Jie, Li, Ruipeng, Grünwald, Michael, and Chen, Ou. Self-Assembly of Quantum Dot–Gold Heterodimer Nanocrystals with Orientational Order. United States: N. p., 2018. Web. doi:10.1021/acs.nanolett.8b01860.
Zhu, Hua, Fan, Zhaochuan, Yuan, Yucheng, Wilson, Mitchell A., Hills-Kimball, Katie, Wei, Zichao, He, Jie, Li, Ruipeng, Grünwald, Michael, & Chen, Ou. Self-Assembly of Quantum Dot–Gold Heterodimer Nanocrystals with Orientational Order. United States. doi:10.1021/acs.nanolett.8b01860.
Zhu, Hua, Fan, Zhaochuan, Yuan, Yucheng, Wilson, Mitchell A., Hills-Kimball, Katie, Wei, Zichao, He, Jie, Li, Ruipeng, Grünwald, Michael, and Chen, Ou. Tue . "Self-Assembly of Quantum Dot–Gold Heterodimer Nanocrystals with Orientational Order". United States. doi:10.1021/acs.nanolett.8b01860. https://www.osti.gov/servlets/purl/1475146.
@article{osti_1475146,
title = {Self-Assembly of Quantum Dot–Gold Heterodimer Nanocrystals with Orientational Order},
author = {Zhu, Hua and Fan, Zhaochuan and Yuan, Yucheng and Wilson, Mitchell A. and Hills-Kimball, Katie and Wei, Zichao and He, Jie and Li, Ruipeng and Grünwald, Michael and Chen, Ou},
abstractNote = {The self-assembly of nanocrystals into ordered superlattices is a powerful strategy for the production of functional nanomaterials. The assembly of well-ordered target structures, however, requires control over the building blocks’ size and shape as well as their interactions. While nanocrystals with homogeneous composition are now routinely synthesized with high precision and assembled into various ordered structures, high-quality multicomponent nanocrystals and their ordered assemblies are rarely reported. In this paper, we demonstrate the synthesis of quantum dot–gold (QD-Au) heterodimers. These heterodimers possess a uniform shape and narrow size distribution and are capped with oleylamine and dodecyltrimethylammonium bromide (DTAB). Assembly of the heterodimers results in a superlattice with long-range orientational alignment of dimers. Using synchrotron-based X-ray measurements, we characterize the complex superstructure formed from the dimers. Molecular dynamics simulations of a coarse-grained model suggest that anisotropic interactions between the quantum dot and gold components of the dimer drive superlattice formation. The high degree of orientational order demonstrated in this work is a potential route to nanomaterials with useful optoelectronic properties.},
doi = {10.1021/acs.nanolett.8b01860},
journal = {Nano Letters},
number = 8,
volume = 18,
place = {United States},
year = {2018},
month = {7}
}

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