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Title: Interparticle spacing and structural ordering in superlattice PbS nanocrystal solids undergoing ligand exchange

Abstract

Controlling the interparticle spacing in quantum dot (QD) thin films is the most readily accessible way to control transport rates between neighboring QDs and a critical component of device optimization. Here, we use X-ray scattering measurements to accurately measure the interparticle spacing in films of highly monodisperse lead sulfide (PbS) QDs that have undergone a variety of device-relevant ligand exchanges. We tabulate these values for use in simulations and data analysis. We find that monothiol and dithiol ligand species typically result in interparticle spacing values that are equal to the length of a single monothiol or dithiol ligand. Additionally, we find that spin-coating a thick film of QDs followed by a long-duration ligand exchange results in a more complete ligand exchange than spin-coating many thin layers with short-duration ligand exchanges in between. The former method also preserves a remarkable degree of the long-range ordering that was present in the film prior to ligand exchange. These results shed light on ways to produce highly-ordered QD solids with compact and functional ligands, which could lead to enhanced interdot coupling and transport phenomena.

Authors:
 [1];  [2];  [1]
  1. MIT (Massachusetts Inst. of Technology), Cambridge, MA (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1183851
Report Number(s):
BNL-107970-2015-JA
Journal ID: ISSN 0897-4756; R&D Project: 16077; KC0403020
Grant/Contract Number:  
SC00112704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 27; Journal Issue: 2; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; functional nanomaterials

Citation Formats

Weidman, Mark C., Yager, Kevin G., and Tisdale, William A. Interparticle spacing and structural ordering in superlattice PbS nanocrystal solids undergoing ligand exchange. United States: N. p., 2014. Web. doi:10.1021/cm503626s.
Weidman, Mark C., Yager, Kevin G., & Tisdale, William A. Interparticle spacing and structural ordering in superlattice PbS nanocrystal solids undergoing ligand exchange. United States. https://doi.org/10.1021/cm503626s
Weidman, Mark C., Yager, Kevin G., and Tisdale, William A. 2014. "Interparticle spacing and structural ordering in superlattice PbS nanocrystal solids undergoing ligand exchange". United States. https://doi.org/10.1021/cm503626s. https://www.osti.gov/servlets/purl/1183851.
@article{osti_1183851,
title = {Interparticle spacing and structural ordering in superlattice PbS nanocrystal solids undergoing ligand exchange},
author = {Weidman, Mark C. and Yager, Kevin G. and Tisdale, William A.},
abstractNote = {Controlling the interparticle spacing in quantum dot (QD) thin films is the most readily accessible way to control transport rates between neighboring QDs and a critical component of device optimization. Here, we use X-ray scattering measurements to accurately measure the interparticle spacing in films of highly monodisperse lead sulfide (PbS) QDs that have undergone a variety of device-relevant ligand exchanges. We tabulate these values for use in simulations and data analysis. We find that monothiol and dithiol ligand species typically result in interparticle spacing values that are equal to the length of a single monothiol or dithiol ligand. Additionally, we find that spin-coating a thick film of QDs followed by a long-duration ligand exchange results in a more complete ligand exchange than spin-coating many thin layers with short-duration ligand exchanges in between. The former method also preserves a remarkable degree of the long-range ordering that was present in the film prior to ligand exchange. These results shed light on ways to produce highly-ordered QD solids with compact and functional ligands, which could lead to enhanced interdot coupling and transport phenomena.},
doi = {10.1021/cm503626s},
url = {https://www.osti.gov/biblio/1183851}, journal = {Chemistry of Materials},
issn = {0897-4756},
number = 2,
volume = 27,
place = {United States},
year = {Fri Dec 12 00:00:00 EST 2014},
month = {Fri Dec 12 00:00:00 EST 2014}
}

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Free Publicly Available Full Text
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Cited by: 94 works
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Works referenced in this record:

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Comparing Halide Ligands in PbS Colloidal Quantum Dots for Field-Effect Transistors and Solar Cells
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Long-Range Order in Nanocrystal Assemblies Determines Charge Transport of Films
journal, July 2017


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