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Title: Ordered Networks of Gold Nanoparticles Crosslinked by Dithiol-Oligomers

Abstract

Here, controlled aggregation of nanoparticles into superlattices is a grand challenge in material science, where ligand based self–assembly is the dominant route. Here, the self–assembly of gold nanoparticles (AuNPs) that are crosslinked by water soluble oligo–(ethylene glycol)–dithiol (oEG–dithiol) is reported and their 3D structure by small angle X–ray scattering is determined. Surprisingly, a narrow region is found in the parameter space of dithiol linker–length and nanoparticle size for which the crosslinked networks form short–ranged FCC crystals. Using geometrical considerations and numerical simulations, the stability of the formed lattices is evaluated as a function of dithiol length and the number of connected nearest–neighbors, and a phase diagram of superlattice formation is provided. Identifying the narrow parameter space that allows crystallization facilitates focused exploration of linker chemical composition and medium conditions such as thermal annealing, pH, and added solutes that may lead to superior and more robust crystals.

Authors:
 [1];  [1];  [1];  [2];  [1];  [1]; ORCiD logo [1]
  1. Ames Lab. and Iowa State Univ., Ames, IA (United States)
  2. Ames Lab., Ames, IA (United States)
Publication Date:
Research Org.:
Ames Laboratory (AMES), Ames, IA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1471220
Alternate Identifier(s):
OSTI ID: 1454899
Report Number(s):
IS-J-9742
Journal ID: ISSN 0934-0866
Grant/Contract Number:  
AC02-07CH11358; AC02-06CH11357; ACI-1548562; TG-MCB14007
Resource Type:
Accepted Manuscript
Journal Name:
Particle & Particle Systems Characterization
Additional Journal Information:
Journal Volume: 35; Journal Issue: 8; Journal ID: ISSN 0934-0866
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; crosslinking method; nanoparticle crystallization; nanoparticle self-assembly; SAXs

Citation Formats

Nayak, Srikanth, Horst, Nathan, Zhang, Honghu, Wang, Wenjie, Mallapragada, Surya, Travesset, Alex, and Vaknin, David. Ordered Networks of Gold Nanoparticles Crosslinked by Dithiol-Oligomers. United States: N. p., 2018. Web. doi:10.1002/ppsc.201800097.
Nayak, Srikanth, Horst, Nathan, Zhang, Honghu, Wang, Wenjie, Mallapragada, Surya, Travesset, Alex, & Vaknin, David. Ordered Networks of Gold Nanoparticles Crosslinked by Dithiol-Oligomers. United States. doi:https://doi.org/10.1002/ppsc.201800097
Nayak, Srikanth, Horst, Nathan, Zhang, Honghu, Wang, Wenjie, Mallapragada, Surya, Travesset, Alex, and Vaknin, David. Tue . "Ordered Networks of Gold Nanoparticles Crosslinked by Dithiol-Oligomers". United States. doi:https://doi.org/10.1002/ppsc.201800097. https://www.osti.gov/servlets/purl/1471220.
@article{osti_1471220,
title = {Ordered Networks of Gold Nanoparticles Crosslinked by Dithiol-Oligomers},
author = {Nayak, Srikanth and Horst, Nathan and Zhang, Honghu and Wang, Wenjie and Mallapragada, Surya and Travesset, Alex and Vaknin, David},
abstractNote = {Here, controlled aggregation of nanoparticles into superlattices is a grand challenge in material science, where ligand based self–assembly is the dominant route. Here, the self–assembly of gold nanoparticles (AuNPs) that are crosslinked by water soluble oligo–(ethylene glycol)–dithiol (oEG–dithiol) is reported and their 3D structure by small angle X–ray scattering is determined. Surprisingly, a narrow region is found in the parameter space of dithiol linker–length and nanoparticle size for which the crosslinked networks form short–ranged FCC crystals. Using geometrical considerations and numerical simulations, the stability of the formed lattices is evaluated as a function of dithiol length and the number of connected nearest–neighbors, and a phase diagram of superlattice formation is provided. Identifying the narrow parameter space that allows crystallization facilitates focused exploration of linker chemical composition and medium conditions such as thermal annealing, pH, and added solutes that may lead to superior and more robust crystals.},
doi = {10.1002/ppsc.201800097},
journal = {Particle & Particle Systems Characterization},
number = 8,
volume = 35,
place = {United States},
year = {2018},
month = {6}
}

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Cited by: 1 work
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Figures / Tables:

Figure 1 Figure 1: Schematic of the procedure to obtain AuNP-dithiol aggregates. AuNPs are cross-linked by short, water soluble dithiols and form superlattices with short-ranged order (SRO).

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Works referenced in this record:

Controlling Structure and Porosity in Catalytic Nanoparticle Superlattices with DNA
journal, January 2015

  • Auyeung, Evelyn; Morris, William; Mondloch, Joseph E.
  • Journal of the American Chemical Society, Vol. 137, Issue 4
  • DOI: 10.1021/ja512116p

Templated Techniques for the Synthesis and Assembly of Plasmonic Nanostructures
journal, June 2011

  • Jones, Matthew R.; Osberg, Kyle D.; Macfarlane, Robert J.
  • Chemical Reviews, Vol. 111, Issue 6
  • DOI: 10.1021/cr1004452

Impact of the Crosslinker’s Molecular Structure on the Aggregation of Gold Nanoparticles
journal, January 2017

  • Deffner, Michael; Schulz, Florian; Lange, Holger
  • Zeitschrift für Physikalische Chemie, Vol. 231, Issue 1
  • DOI: 10.1515/zpch-2016-0865

Phase diagram of power law and Lennard-Jones systems: Crystal phases
journal, October 2014

  • Travesset, Alex
  • The Journal of Chemical Physics, Vol. 141, Issue 16
  • DOI: 10.1063/1.4898371

Understanding interactions between capped nanocrystals: Three-body and chain packing effects
journal, September 2009

  • Schapotschnikow, Philipp; Vlugt, Thijs J. H.
  • The Journal of Chemical Physics, Vol. 131, Issue 12
  • DOI: 10.1063/1.3227043

DNA-guided crystallization of colloidal nanoparticles
journal, January 2008

  • Nykypanchuk, Dmytro; Maye, Mathew M.; van der Lelie, Daniel
  • Nature, Vol. 451, Issue 7178, p. 549-552
  • DOI: 10.1038/nature06560

Novel gold-dithiol nano-networks with non-metallic electronic properties
journal, September 1995

  • Brust, Mathias; Schiffrin, David J.; Bethell, Donald
  • Advanced Materials, Vol. 7, Issue 9
  • DOI: 10.1002/adma.19950070907

Establishing the Design Rules for DNA-Mediated Programmable Colloidal Crystallization
journal, May 2010

  • Macfarlane, Robert J.; Jones, Matthew R.; Senesi, Andrew J.
  • Angewandte Chemie International Edition, Vol. 49, Issue 27
  • DOI: 10.1002/anie.201000633

Small is different: energetic, structural, thermal, and mechanical properties of passivated nanocluster assemblies
journal, January 2004

  • Landman, Uzi; Luedtke, W. D.
  • Faraday Discussions, Vol. 125
  • DOI: 10.1039/b312640b

Topological structure prediction in binary nanoparticle superlattices
journal, January 2017


Self-assembled plasmonic nanostructures
journal, January 2014

  • Klinkova, Anna; Choueiri, Rachelle M.; Kumacheva, Eugenia
  • Chemical Society Reviews, Vol. 43, Issue 11
  • DOI: 10.1039/c3cs60341e

Interparticle Forces Underlying Nanoparticle Self-Assemblies
journal, October 2015


DNA-nanoparticle superlattices formed from anisotropic building blocks
journal, October 2010

  • Jones, Matthew R.; Macfarlane, Robert J.; Lee, Byeongdu
  • Nature Materials, Vol. 9, Issue 11, p. 913-917
  • DOI: 10.1038/nmat2870

Capping Ligand Vortices as “Atomic Orbitals” in Nanocrystal Self-Assembly
journal, September 2017


Gold Nanorods to Nanochains:  Mechanistic Investigations on Their Longitudinal Assembly Using α,ω-Alkanedithiols and Interplasmon Coupling
journal, January 2006

  • Shibu Joseph, S. T.; Ipe, Binil Itty; Pramod, P.
  • The Journal of Physical Chemistry B, Vol. 110, Issue 1
  • DOI: 10.1021/jp0544179

Self-Assembly at All Scales
journal, March 2002

  • Whitesides, George M.; Grzybowski, Bartosz
  • Science, Vol. 295, Issue 5564, p. 2418-2421
  • DOI: 10.1126/science.1070821

[INVITED] Self-assembled optical metamaterials
journal, August 2016


Assembling and ordering polymer-grafted nanoparticles in three dimensions
journal, January 2017

  • Zhang, Honghu; Wang, Wenjie; Akinc, Mufit
  • Nanoscale, Vol. 9, Issue 25
  • DOI: 10.1039/C7NR00787F

Formation of Spherical Nanostructures by the Controlled Aggregation of Gold Colloids
journal, March 2006

  • Hussain, Irshad; Wang, Zhenxin; Cooper, Andrew I.
  • Langmuir, Vol. 22, Issue 7
  • DOI: 10.1021/la053126o

A DNA-based method for rationally assembling nanoparticles into macroscopic materials
journal, August 1996

  • Mirkin, Chad A.; Letsinger, Robert L.; Mucic, Robert C.
  • Nature, Vol. 382, Issue 6592, p. 607-609
  • DOI: 10.1038/382607a0

Micellar crystals in solution from molecular dynamics simulations
journal, May 2008

  • Anderson, J. A.; Lorenz, C. D.; Travesset, A.
  • The Journal of Chemical Physics, Vol. 128, Issue 18
  • DOI: 10.1063/1.2913522

Carbon-coated nanoparticle superlattices for energy applications
journal, January 2016

  • Li, Jun; Yiliguma, Yiliguma; Wang, Yifei
  • Nanoscale, Vol. 8, Issue 30
  • DOI: 10.1039/C6NR03243E

Electrolyte-Mediated Assembly of Charged Nanoparticles
journal, April 2016

  • Kewalramani, Sumit; Guerrero-García, Guillermo I.; Moreau, Liane M.
  • ACS Central Science, Vol. 2, Issue 4
  • DOI: 10.1021/acscentsci.6b00023

Macroscopic and tunable nanoparticle superlattices
journal, January 2017

  • Zhang, Honghu; Wang, Wenjie; Mallapragada, Surya
  • Nanoscale, Vol. 9, Issue 1
  • DOI: 10.1039/C6NR07136H

Two-Dimensional DNA-Programmable Assembly of Nanoparticles at Liquid Interfaces
journal, May 2014

  • Srivastava, Sunita; Nykypanchuk, Dmytro; Fukuto, Masafumi
  • Journal of the American Chemical Society, Vol. 136, Issue 23
  • DOI: 10.1021/ja501749b

General purpose molecular dynamics simulations fully implemented on graphics processing units
journal, May 2008

  • Anderson, Joshua A.; Lorenz, Chris D.; Travesset, A.
  • Journal of Computational Physics, Vol. 227, Issue 10
  • DOI: 10.1016/j.jcp.2008.01.047

Scattering Curves of Ordered Mesoscopic Materials
journal, February 2005

  • Förster, S.; Timmann, A.; Konrad, M.
  • The Journal of Physical Chemistry B, Vol. 109, Issue 4
  • DOI: 10.1021/jp0467494

Nanoparticleassemblies for biological and chemical sensing
journal, January 2010

  • Liu, Shaoqin; Tang, Zhiyong
  • J. Mater. Chem., Vol. 20, Issue 1
  • DOI: 10.1039/B911328M

Crystallization of DNA-Capped Gold Nanoparticles in High-Concentration, Divalent Salt Environments
journal, December 2013

  • Tan, Shawn J.; Kahn, Jason S.; Derrien, Thomas L.
  • Angewandte Chemie International Edition, Vol. 53, Issue 5
  • DOI: 10.1002/anie.201307113

Determining the composition of gold nanoparticles: a compilation of shapes, sizes, and calculations using geometric considerations
journal, October 2016


Charge Transport in Nanoparticle Assemblies
journal, October 2008

  • Zabet-Khosousi, Amir; Dhirani, Al-Amin
  • Chemical Reviews, Vol. 108, Issue 10
  • DOI: 10.1021/cr0680134

Molecular control over colloidal assembly
journal, January 2017

  • Gerth, M.; Voets, I. K.
  • Chemical Communications, Vol. 53, Issue 32
  • DOI: 10.1039/C6CC09985H

Nanoparticle Superlattice Engineering with DNA
journal, October 2011


Directed Self-Assembly of Nanoparticles
journal, June 2010

  • Grzelczak, Marek; Vermant, Jan; Furst, Eric M.
  • ACS Nano, Vol. 4, Issue 7
  • DOI: 10.1021/nn100869j

Hydrogen Bonding Stabilized Self-Assembly of Inorganic Nanoparticles: Mechanism and Collective Properties
journal, May 2015


Controllable formation and TEM spatial visualization of cross-linked gold nanoparticle spherical aggregates
journal, January 2011

  • Lin, Guangyao; Wang, Yong; Zhang, Qianjun
  • Nanoscale, Vol. 3, Issue 11
  • DOI: 10.1039/c1nr10897b

The Structure of Gold-Nanoparticle Networks Cross-Linked by Di- and Multifunctional RAFT Oligomers
journal, September 2015


Gold Nanoparticle Based FRET for DNA Detection
journal, August 2007


Gold Nanorod Linking to Control Plasmonic Properties in Solution and Polymer Nanocomposites
journal, February 2014

  • Ferrier, Robert C.; Lee, Hyun-Su; Hore, Michael J. A.
  • Langmuir, Vol. 30, Issue 7
  • DOI: 10.1021/la404588w

Strong scaling of general-purpose molecular dynamics simulations on GPUs
journal, July 2015

  • Glaser, Jens; Nguyen, Trung Dac; Anderson, Joshua A.
  • Computer Physics Communications, Vol. 192
  • DOI: 10.1016/j.cpc.2015.02.028

DNA-programmable nanoparticle crystallization
journal, January 2008

  • Park, Sung Yong; Lytton-Jean, Abigail K. R.; Lee, Byeongdu
  • Nature, Vol. 451, Issue 7178, p. 553-556
  • DOI: 10.1038/nature06508

Self-assembly of nanoparticles into structured spherical and network aggregates
journal, April 2000

  • Boal, Andrew K.; Ilhan, Faysal; DeRouchey, Jason E.
  • Nature, Vol. 404, Issue 6779
  • DOI: 10.1038/35008037

A parameter-free, solid-angle based, nearest-neighbor algorithm
journal, June 2012

  • van Meel, Jacobus A.; Filion, Laura; Valeriani, Chantal
  • The Journal of Chemical Physics, Vol. 136, Issue 23
  • DOI: 10.1063/1.4729313

Synthesis and optical properties of gold nanoparticle networks cross-linked with chain-length-controlled polymers
journal, January 2015


Rigid body constraints realized in massively-parallel molecular dynamics on graphics processing units
journal, November 2011

  • Nguyen, Trung Dac; Phillips, Carolyn L.; Anderson, Joshua A.
  • Computer Physics Communications, Vol. 182, Issue 11
  • DOI: 10.1016/j.cpc.2011.06.005

Small-angle scattering of particle assemblies
journal, July 2015


Prospects of Colloidal Nanocrystals for Electronic and Optoelectronic Applications
journal, January 2010

  • Talapin, Dmitri V.; Lee, Jong-Soo; Kovalenko, Maksym V.
  • Chemical Reviews, Vol. 110, Issue 1
  • DOI: 10.1021/cr900137k

Properties and emerging applications of self-assembled structures made from inorganic nanoparticles
journal, December 2009

  • Nie, Zhihong; Petukhova, Alla; Kumacheva, Eugenia
  • Nature Nanotechnology, Vol. 5, Issue 1
  • DOI: 10.1038/nnano.2009.453

Challenges in fabrication towards realization of practical metamaterials
journal, September 2016


Self-Assembly of Colloidal Nanocrystals: From Intricate Structures to Functional Materials
journal, August 2016


Crystalline Gibbs Monolayers of DNA-Capped Nanoparticles at the Air–Liquid Interface
journal, September 2011

  • Campolongo, Michael J.; Tan, Shawn J.; Smilgies, Detlef-M.
  • ACS Nano, Vol. 5, Issue 10
  • DOI: 10.1021/nn202383b

Gold nanoparticle superlattices
journal, January 2008

  • Prasad, B. L. V.; Sorensen, C. M.; Klabunde, Kenneth J.
  • Chemical Society Reviews, Vol. 37, Issue 9
  • DOI: 10.1039/b712175j