3 years ago

Nanophase Segregation of Self-Assembled Monolayers on Gold Nanoparticles

Nanophase Segregation of Self-Assembled Monolayers on Gold Nanoparticles
David Portehault, Ovidiu Ersen, Simona Moldovan, François Ribot, Clément Sanchez, Claire Goldmann, Santosh Kumar Meena, Thomas Marchandier, Douga Nassoko, Marialore Sulpizi, Mahamadou Seydou, Corinne Chanéac, Frederik Tielens
Nanophase segregation of a bicomponent thiol self-assembled monolayer is predicted using atomistic molecular dynamics simulations and experimentally confirmed. The simulations suggest the formation of domains rich in acid-terminated chains, on one hand, and of domains rich in amide-functionalized ethylene glycol oligomers, on the other hand. In particular, within the amide-ethylene glycol oligomers region, a key role is played by the formation of interchain hydrogen bonds. The predicted phase segregation is experimentally confirmed by the synthesis of 35 and 15 nm gold nanoparticles functionalized with several binary mixtures of ligands. An extensive study by transmission electron microscopy and electron tomography, using silica selective heterogeneous nucleation on acid-rich domains to provide electron contrast, supports simulations and highlights patchy nanoparticles with a trend toward Janus nano-objects depending on the nature of the ligands and the particle size. These results validate our computational platform as an effective tool to predict nanophase separation in organic mixtures on a surface and drive further exploration of advanced nanoparticle functionalization.

Publisher URL: http://dx.doi.org/10.1021/acsnano.7b03616

DOI: 10.1021/acsnano.7b03616

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