Bidisperse Nanospheres Jammed on a Liquid Surface

Jammed packings of bidisperse nanospheres were assembled on a nonvolatile liquid surface and visualized to the single-particle scale by using an in situ scanning electron microscopy method. The PEGylated silica nanospheres, mixed at different number fractions and size ratios, had large enough in-plane mobilities prior to jamming to form uniform monolayers reproducibly. From the collected nanometer-resolution images, local order and degree of mixing were assessed by standard metrics. For equimolar mixtures, a large-to-small size ratio of about 1.5 minimized correlated metrics for local orientational and positional order, as previously predicted in simulations of bidisperse disk jamming. Despite monolayer uniformity, structural and depletion interactions caused spheres of a similar size to cluster, a feature evident at size ratios above 2. Uniform nanoparticle monolayers of high packing disorder are sought in many liquid interface technologies, and these experiments outlined key design principles, buttressing extensive theory/simulation literature on the topic.