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Controlled Self-Assembly and Tuning of Large PbS Nanoparticle Supercrystals

Journal Article · · Chemistry of Materials
 [1];  [2];  [3]
  1. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). NSLS II
  3. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Center for Integrated Nanotechnologies; Univ. of New Mexico, Albuquerque, NM (United States). Dept. of Chemical and Biological Engineering. Center for Micro-Engineered Materials

Self-assembly of colloidal nanocrystals (NCs) into ordered superlattices (SLs) and supercrystals (SCs) enables new artificial NC solids for nanoelectronic and nanophotonic applications, which requires critical control of nucleation and growth conditions. In this paper, large SCs of PbS NCs up to ~100 μm size were synthesized by two controlled self-assembly methods from NC solutions. Both translational symmetry and orientational ordering of the nanocrystals in the SCs were readily tuned by excess oleic acid ligands and antisolvents. Slow evaporation and the counterdiffusion method of solvents resulted in the formation of single SCs with two different SLs from the same PbS NCs: a face-centered cubic SL with weak yet complex orientational order or a body-centered cubic SL with strong and uniform particle orientation, respectively. The translational ordering was mainly determined by the effective shape of the NCs while the difference in orientational order was a result of the balance between ligand–ligand attraction and rotational entropy. Finally, the ease of the growth of large SC solids could lead to diverse NC systems and facilitate essential investigation of nanoparticle interactions and coupling based nanoelectronic and nanophotonic properties.

Research Organization:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE National Nuclear Security Administration (NNSA); SNL Laboratory Directed Research and Development (LDRD) Program
Grant/Contract Number:
NA0003525
OSTI ID:
1474085
Alternate ID(s):
OSTI ID: 1477956
Report Number(s):
SAND--2018-10292J; 668023
Journal Information:
Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 19 Vol. 30; ISSN 0897-4756
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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Cited By (8)

Hierarchical supercrystalline nanocomposites through the self-assembly of organically-modified ceramic nanoparticles text January 2019
Supercrystallography-Based Decoding of Structure and Driving Force of Nanocrystal Assembly journal November 2019
Oriented Gold Nanorod Arrays: Self‐Assembly and Optoelectronic Applications journal June 2019
Oriented Gold Nanorod Arrays: Self-Assembly and Optoelectronic Applications journal June 2019
Collective topo-epitaxy in the self-assembly of a 3D quantum dot superlattice journal October 2019
Hierarchical supercrystalline nanocomposites through the self-assembly of organically-modified ceramic nanoparticles journal March 2019
In situ formation of electronically coupled superlattices of Cu 1.1 S nanodiscs at the liquid/air interface journal January 2019
Tunable electronic properties by ligand coverage control in PbS nanocrystal assemblies journal January 2019

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