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Nanoparticles are often covered in ligand monolayers, which can undergo atemperature-dependent order-disorder transition that switches theparticle-particle interaction from repulsive to attractive in solution. In thiswork, we examine how changes in the ligand surface coverage and facetdimensions affect the ordering of ligands, the arrangement of nearby solventmolecules, and the interaction between ligand monolayers on differentparticles. In particular, we consider the case of strongly bound octadecylligands on the (100) facet of CdS in the presence of an explicit n-hexanesolvent. Depending on the facet dimensions and surface coverage, we observethree distinct ordered states that differ in how the ligands are packedtogether, and which affect the thickness of the ligand shell and the structureof the ligand-solvent interface. The temperature dependence of theorder-disorder transition also broadens and shifts to lower temperature in anonlinear manner as the nanoscale is approached from above. We find thatligands on nanoscale facets can behave very similarly to those on macroscopicsurfaces in solution, and that some facet dimensions affect the ligandalignment more strongly than others. As the ligands order, the interactionbetween opposing monolayers becomes attractive, even well below full surfacecoverage. The strength of attraction per unit surface area is strongly affectedby ligand coverage, but only weakly by facet width. Conversely, we find thatbringing two monolayers together just above the order-disorder transitiontemperature can induce ordering and attraction.

Ligand-Mediated Interactions between Nanoscale Surfaces Depend Sensitively and Nonlinearly on Temperature, Facet Dimensions, and Ligand Coverage