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Solvent plays an important role in the relative motion of nanoscopic bodies,and the study of such phenomena can help elucidate the mechanism of hydrophobicassembly, as well as the influence of solvent-mediated effects on in vivomotion in crowded cellular environments. Here we study important aspects ofthis problem within the framework of Brownian dynamics. We compute the freeenergy surface that the Brownian particles experience and their hydrodynamicinteractions from molecular dynamics simulations in explicit solvent. We findthat molecular scale effects dominate at short distances, thus giving rise todeviations from the predictions of continuum hydrodynamic theory. Dryingphenomena, solvent layering, and fluctuations engender distinct signatures ofthe molecular scale. The rate of assembly in the diffusion-controlled limit isfound to decrease from molecular scale hydrodynamic interactions, in oppositionto the free energy driving force for hydrophobic assembly, and act to reinforcethe influence of the free energy surface on the association of more hydrophilicbodies.

Interplay between hydrodynamics and the free energy surface in the assembly of nanoscale hydrophobes