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Title: Ligand structure and mechanical properties of single-nanoparticle thick membranes

Abstract

We believe that the high mechanical stiffness of single-nanoparticle-thick membranes is the result of the local structure of ligand coatings that mediate interactions between nanoparticles. These ligand structures are not directly observable experimentally. We use molecular dynamics simulations to observe variations in ligand structure and simultaneously measure variations in membrane mechanical properties. We have shown previously that ligand end group has a large impact on ligand structure and membrane mechanical properties. Here we introduce and apply quantitative molecular structure measures to these membranes and extend analysis to multiple nanoparticle core sizes and ligand lengths. Simulations of nanoparticle membranes with a nanoparticle core diameter of 4 or 6 nm, a ligand length of 11 or 17 methylenes, and either carboxyl (COOH) or methyl (CH3) ligand end groups are presented. In carboxyl-terminated ligand systems, structure and interactions are dominated by an end-to-end orientation of ligands. In methyl-terminated ligand systems large ordered ligand structures form, but nanoparticle interactions are dominated by disordered, partially interdigitated ligands. Core size and ligand length also affect both ligand arrangement within the membrane and the membrane's macroscopic mechanical response, but are secondary to the role of the ligand end group. Additionally, the particular end group (COOH or CH3)more » alters the nature of how ligand length, in turn, affects the membrane properties. The effect of core size does not depend on the ligand end group, with larger cores always leading to stiffer membranes. Asymmetry in the stress and ligand density is observed in membranes during preparation at a water-vapor interface, with the stress asymmetry persisting in all membranes after drying.« less

Authors:
 [1];  [1];  [1];  [1]
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  1. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1235281
Alternate Identifier(s):
OSTI ID: 1184884
Report Number(s):
SAND-2015-1157J
Journal ID: ISSN 1539-3755; 567065
Grant/Contract Number:  
AC04-94AL85000
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review. E, Statistical, Nonlinear, and Soft Matter Physics
Additional Journal Information:
Journal Volume: 91; Journal Issue: 06; Journal ID: ISSN 1539-3755
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Salerno, Kenneth Michael, Bolintineanu, Dan S., Lane, J. Matthew D., and Grest, Gary S. Ligand structure and mechanical properties of single-nanoparticle thick membranes. United States: N. p., 2015. Web. doi:10.1103/PhysRevE.91.062403.
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Salerno, Kenneth Michael, Bolintineanu, Dan S., Lane, J. Matthew D., & Grest, Gary S. Ligand structure and mechanical properties of single-nanoparticle thick membranes. United States. https://doi.org/10.1103/PhysRevE.91.062403
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Salerno, Kenneth Michael, Bolintineanu, Dan S., Lane, J. Matthew D., and Grest, Gary S. Tue . "Ligand structure and mechanical properties of single-nanoparticle thick membranes". United States. https://doi.org/10.1103/PhysRevE.91.062403. https://www.osti.gov/servlets/purl/1235281.
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@article{osti_1235281,
title = {Ligand structure and mechanical properties of single-nanoparticle thick membranes},
author = {Salerno, Kenneth Michael and Bolintineanu, Dan S. and Lane, J. Matthew D. and Grest, Gary S.},
abstractNote = {We believe that the high mechanical stiffness of single-nanoparticle-thick membranes is the result of the local structure of ligand coatings that mediate interactions between nanoparticles. These ligand structures are not directly observable experimentally. We use molecular dynamics simulations to observe variations in ligand structure and simultaneously measure variations in membrane mechanical properties. We have shown previously that ligand end group has a large impact on ligand structure and membrane mechanical properties. Here we introduce and apply quantitative molecular structure measures to these membranes and extend analysis to multiple nanoparticle core sizes and ligand lengths. Simulations of nanoparticle membranes with a nanoparticle core diameter of 4 or 6 nm, a ligand length of 11 or 17 methylenes, and either carboxyl (COOH) or methyl (CH3) ligand end groups are presented. In carboxyl-terminated ligand systems, structure and interactions are dominated by an end-to-end orientation of ligands. In methyl-terminated ligand systems large ordered ligand structures form, but nanoparticle interactions are dominated by disordered, partially interdigitated ligands. Core size and ligand length also affect both ligand arrangement within the membrane and the membrane's macroscopic mechanical response, but are secondary to the role of the ligand end group. Additionally, the particular end group (COOH or CH3) alters the nature of how ligand length, in turn, affects the membrane properties. The effect of core size does not depend on the ligand end group, with larger cores always leading to stiffer membranes. Asymmetry in the stress and ligand density is observed in membranes during preparation at a water-vapor interface, with the stress asymmetry persisting in all membranes after drying.},
doi = {10.1103/PhysRevE.91.062403},
journal = {Physical Review. E, Statistical, Nonlinear, and Soft Matter Physics},
number = 06,
volume = 91,
place = {United States},
year = {Tue Jun 16 00:00:00 EDT 2015},
month = {Tue Jun 16 00:00:00 EDT 2015}
}
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https://doi.org/10.1103/PhysRevE.91.062403
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