Asymmetric assembly of Lennard-Jones Janus dimers.

Self-assembly of Janus (or "patchy") particles is dependent on the precise interaction between neighboring particles. Here, the orientations of two amphiphilic Janus spheres within a dimer in an explicit fluid are studied with high geometric resolution. Molecular dynamics simulations and semianalytical energy calculations are used with hard- and soft-sphere Lennard-Jones potentials, and temperature and hydrophobicity are varied. The most probable center-center-pole angles are in the range of 40^{∘}-55^{∘} with pole-to-pole alignment not observed due to orientational entropy. Angles near 90^{∘} are energetically unfavored due to solvent exclusion, and the relative azimuthal angle between the spheres is affected by solvent ordering. Relatively large polar angles become more favored as the hydrophobic surface area (i.e., Janus balance) is increased.

Stability of amphiphilic Janus dimers in shear flow: a molecular dynamics study.

Amphiphilic Janus particles in a flow are thought to experience a torque due to the asymmetry in slip at their surfaces. This effect has the potential to destabilise self-assembled Janus structures in flows due to the forces and torques applied to individual Janus nanoparticles. In this work, we investigate the stability of amphiphilic Janus dimers and homogeneous hydrophobic dimers in shear flow using molecular dynamics, and study possible break-up mechanisms. In particular, we consider the influence of the activation enthalpy and entropy on the thermal break-up rate of these dimers. Janus dimers are less stable than hydrophobic dimers, and increasing the applied shear rate has a greater effect on break-up for Janus dimers. Two mechanisms leading to increased break-up in shear flow are studied, namely the rotational speed of the dimers and the orientation of individual spheres in the dimers, and we propose a descriptive equation for calculation of the break-up rate. Overall, the results indicate that the stability of dimers in shear flow depends on the slip length at the spheres' surfaces, and that the slip length difference on Janus dimers could contribute to destabilisation.

Molecular dynamics simulations of Janus nanoparticles in a fluid flow.

We study the forces and torques on individual Janus nanoparticles in a fluid flow using molecular dynamics simulations. In particular, we consider amphiphilic Janus nanospheres that have different slip boundary conditions on each hemisphere, and calculate the forces and torques experienced by them as a function of their orientation with respect to the flow direction. Furthermore, we examine nanoparticles that are deformed slightly from a spherical shape, and have no-slip boundary conditions. We compare the simulation results to the predictions of previously introduced theoretical approaches, which compute the forces and torques on particles with variable slip lengths or aspherical deformations that are much smaller than the particle radius. We found that there is good qualitative agreement between the forces and torques computed from our simulations and the theoretical predictions, and the forces quantitatively agree when the assumptions made in the theoretical descriptions are satisfied.