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Effect of mesogenic corona on type and anisotropy of gold nanoparticle superlattice: When can tail wag the dog?

The correlation between size of nanoparticles and structure and shape of mesogenic ligands and the ensuing assembly behaviour is not really understood and closer inspection shows very surprising features. Here 2 and 4 nm gold nanoparticles (NP) were synthesized, grafted with a forked ligand containing two rod-like mesogens in its two branches: one with cholesterol and the other with azobenzene. The 4 nm NPs also contained n-hexylthiol as co-ligand. They were found to form an FCC cubic superlattice, while the 2 nm NPs form hexagonal HCP with weak birefringence, hence with partially oriented ligands. The structures were compared with those of related systems containing a range of different azobenzene-to-cholesterol ratios, all giving body-centered tetragonal superlattices with various degrees of anisotropy. Geometric analysis is presented in terms of asphericity of NP surrounding, requirement for space-filling and structural anisotropy. Some general rules are derived to help design the soft corona around the NPs in order to obtain superlattices with desired structure and anisotropy.

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