Synthesis of {111}-faceted au nanocrystals mediated by polyvinylpyrrolidone: Insights from density-functional theory and molecular dynamics

Shih Hsien Liu, Wissam A. Saidi, Ya Zhou, Kristen Ann Fichthorn

Research output: Contribution to journalArticle

19 Citations (Scopus)

Abstract

We use density-functional theory (DFT) and molecular dynamics (MD) to resolve the role of polyvinylpyrrolidone (PVP) in the shape-selective synthesis of Au nanostructures. Using DFT, we probe the adsorption-induced surface energies and spatially resolved binding of PVP monomer analogs on Au(111), Au(100), and (5 × 1) Au(100)-hex. These calculations suggest that {111} facets should be prevalent in Au nanostructures grown with the help of PVP. We explore the role of solvent and find that, while solvent weakens binding, it does not change the trends we observe in vacuum. We fit an ad hoc interatomic potential to the DFT results so we can describe the binding of PVP to the Au surfaces. Using MD simulations based on this potential, we investigate the PVP-induced surface energies, PVP binding affinities, and oxygen density profile of atactic PVP icosamers on Au(111) and (5 × 1) Au(100)-hex. We conclude that {111}-faceted Au nanocrystals are preferred in PVP-mediated synthesis of Au nanostructures. The reconstruction of Au(100) is important in achieving {111}-facet selectivity.

Original languageEnglish (US)
Pages (from-to)11982-11990
Number of pages9
JournalJournal of Physical Chemistry C
Volume119
Issue number21
DOIs
StatePublished - May 28 2015

Fingerprint

Povidone
Nanocrystals
Density functional theory
Molecular dynamics
Nanostructures
nanocrystals
molecular dynamics
density functional theory
Interfacial energy
synthesis
surface energy
flat surfaces
Monomers
Vacuum
affinity
Adsorption
Oxygen
monomers
selectivity
Computer simulation

All Science Journal Classification (ASJC) codes

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films

Cite this

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abstract = "We use density-functional theory (DFT) and molecular dynamics (MD) to resolve the role of polyvinylpyrrolidone (PVP) in the shape-selective synthesis of Au nanostructures. Using DFT, we probe the adsorption-induced surface energies and spatially resolved binding of PVP monomer analogs on Au(111), Au(100), and (5 × 1) Au(100)-hex. These calculations suggest that {111} facets should be prevalent in Au nanostructures grown with the help of PVP. We explore the role of solvent and find that, while solvent weakens binding, it does not change the trends we observe in vacuum. We fit an ad hoc interatomic potential to the DFT results so we can describe the binding of PVP to the Au surfaces. Using MD simulations based on this potential, we investigate the PVP-induced surface energies, PVP binding affinities, and oxygen density profile of atactic PVP icosamers on Au(111) and (5 × 1) Au(100)-hex. We conclude that {111}-faceted Au nanocrystals are preferred in PVP-mediated synthesis of Au nanostructures. The reconstruction of Au(100) is important in achieving {111}-facet selectivity.",
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Synthesis of {111}-faceted au nanocrystals mediated by polyvinylpyrrolidone : Insights from density-functional theory and molecular dynamics. / Liu, Shih Hsien; Saidi, Wissam A.; Zhou, Ya; Fichthorn, Kristen Ann.

In: Journal of Physical Chemistry C, Vol. 119, No. 21, 28.05.2015, p. 11982-11990.

Research output: Contribution to journalArticle

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