Multicomponent nanoparticle superlattices (SLs) promise the integration of nanoparticles (NPs) with remarkable electronic, magnetic, and optical properties into a single structure. Here we demonstrate that heterodimers consisting of two conjoined NPs can self-assemble into novel multicomponent SLs exhibiting a high degree of alignment between the atomic lattices of individual NPs, which has been theorized to lead to a wide variety of remarkable properties. Specifically, by using simulations and experiments, we find that heterodimers composed of larger Fe3O4 domains decorated with a Pt domain at one vertex will self-assemble into an SL with long-range atomic alignment between the Fe3O4 domains of different NPs across the SL . In-situ scattering of the self-assembly reveals the two-stages mechanism of self-assembly that atomic alignment occurs after developing translational order between NPs. The SLs show an unanticipated decreased coercivity relative to non-assembled NPs. Our results indicate that the atomic alignment is driven by particle shape and is thus composition independent, making the assembly principles generally applicable to the future preparation of multicomponent materials with fine structural control.

Self-assembly of atomically aligned nanoparticle superlattices from Pt-Fe3O4heterodimer-nanoparticles

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