Materials by design for stiff and tough hairy nanoparticle assemblies

Nitin K. Hansoge, Tianyu Huang, Robert Sinko, Wenjie Xia, Wei Chen, Sinan Keten*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

37 Scopus citations


Matrix-free polymer-grafted nanocrystals, called assembled hairy nanoparticles (aHNPs), can significantly enhance the thermomechanical performance of nanocomposites by overcoming nanoparticle dispersion challenges and achieving stronger interfacial interactions through grafted polymer chains. However, effective strategies to improve both the mechanical stiffness and toughness of aHNPs are lacking given the general conflicting nature of these two properties and the large number of molecular parameters involved in the design of aHNPs. Here, we propose a computational framework that combines multiresponse Gaussian process metamodeling and coarse-grained molecular dynamics simulations to establish design strategies for achieving optimal mechanical properties of aHNPs within a parametric space. Taking poly(methyl methacrylate) grafted to high-aspect-ratio cellulose nanocrystals as a model nanocomposite, our multiobjective design optimization framework reveals that the polymer chain length and grafting density are the main influencing factors governing the mechanical properties of aHNPs, in comparison to the nanoparticle size and the polymer-nanoparticle interfacial interactions. In particular, the Pareto frontier, that marks the upper bound of mechanical properties within the design parameter space, can be achieved when the weight percentage of nanoparticles is above around 60% and the grafted chains exceed the critical length scale governing transition into the semidilute brush regime. We show that theoretical scaling relationships derived from the Daoud-Cotton model capture the dependence of the critical length scale on graft density and nanoparticle size. Our established modeling framework provides valuable insights into the mechanical behavior of these hairy nanoparticle assemblies at the molecular level and allows us to establish guidelines for nanocomposite design.

Original languageEnglish (US)
Pages (from-to)7946-7958
Number of pages13
JournalACS nano
Issue number8
StatePublished - Aug 28 2018


  • Pareto frontier
  • assembled hairy nanoparticles
  • coarse-grained molecular dynamics
  • mechanical properties
  • multiresponse Gaussian process modeling

ASJC Scopus subject areas

  • Materials Science(all)
  • Engineering(all)
  • Physics and Astronomy(all)


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