Influence of Fluctuating Membranes on Self-Assembly of Patchy Colloids

A coarse-grained computational model is used to investigate the effect of a fluid membrane on patchy-particle assembly into biologically-relevant structures motivated by viral cores and clathrin. For cores, we demonstrate a non-monotonic dependence of the promotion of assembly on membrane stiffness. If the membrane is significantly deformable, cores are enveloped in buds, although this effect is suppressed for very flexible membranes. In the less deformable regime, we observe no marked enhancement for cores, even for strong adhesion to the surface. For clarthrin-like particles, we again observe the formation of buds, whose morphology depends on membrane-flexibility.Comment: 20 pages, 8 figures, accepted for publication in PRL (http://prl.aps.org

Diffusion and Relaxation Dynamics in Cluster Crystals

For a large class of fluids exhibiting ultrasoft bounded pair potentials, particles form crystals consisting of clusters located in the lattice sites, with a density-independent lattice constant. Here we present an investigation on the dynamic features of a representative example of this class. It is found that particles can diffuse between lattice sites, maintaining the lattice structure, through an activated hopping mechanism. This feature yields finite values for the diffusivity and full relaxation of density correlation functions. Simulations suggest the existence of a localization transition which is avoided by hopping, and a dynamic decoupling between self- and collective correlations.Comment: 4 pages, 7 figure

Soft self-assembled nanoparticles with temperature-dependent properties

The fabrication of versatile building blocks that are reliably self-assemble into desired ordered and disordered phases is amongst the hottest topics in contemporary material science. To this end, microscopic units of varying complexity, aimed at assembling the target phases, have been thought, designed, investigated and built. Such a path usually requires laborious fabrication techniques, especially when a specific funcionalisation of the building blocks is required. Telechelic star polymers, i.e., star polymers made of a number $f$ of di-block copolymers consisting of solvophobic and solvophilic monomers grafted on a central anchoring point, spontaneously self-assemble into soft patchy particles featuring attractive spots (patches) on the surface. Here we show that the tunability of such a system can be widely extended by controlling the physical and chemical parameters of the solution. Indeed, at fixed external conditions the self-assembly behaviour depends only on the number of arms and/or on the ratio of solvophobic to solvophilic monomers. However, changes in temperature and/or solvent quality makes it possible to reliably change the number and size of the attractive patches. This allows to steer the mesoscopic self-assembly behaviour without modifying the microscopic constituents. Interestingly, we also demonstrate that diverse combinations of the parameters can generate stars with the same number of patches but different radial and angular stiffness. This mechanism could provide a neat way of further fine-tuning the elastic properties of the supramolecular network without changing its topology.Comment: 8 pages, 7 figures. Submitted to Nanoscal

Equilibrium properties of highly asymmetric star-polymer mixtures

We employ effective interaction potentials to study the equilibrium structure and phase behavior of highly asymmetric mixtures of star polymers. We consider in particular the influence of the addition of a component with a small number of arms and a small size on a concentrated solution of large stars with a high functionality. By employing liquid integral equation theories we examine the evolution of the correlation functions of the big stars upon addition of the small ones, finding a loss of structure that can be attributed to a weakening of the repulsions between the large stars due to the presence of the small ones. We analyze this phenomenon be means of a generalized depletion mechanism which is supported by computer simulations. By applying thermodynamic perturbation theory we draw the phase diagram of the asymmetric mixture, finding that the addition of small stars melts the crystal formed by the big ones. A systematic comparison between the two- and effective one-component descriptions of the mixture that corroborates the reliability of the generalized depletion picture is also carried out.Comment: 26 pages, 9 figures, submitted to Phys. Rev.

Soft effective interactions between weakly charged polyelectrolyte chains

We apply extensive Molecular Dynamics simulations and analytical considerations in order to study the conformations and the effective interactions between weakly charged, flexible polyelectrolyte chains in salt-free conditions. We focus on charging fractions lying below 20%, for which case there is no Manning condensation of counterions and the latter can be thus partitioned in two states: those that are trapped within the region of the flexible chain and the ones that are free in the solution. We examine the partition of counterions in these two states, the chain sizes and the monomer distributions for various chain lengths, finding that the monomer density follows a Gaussian shape. We calculate the effective interaction between the centers of mass of two interacting chains, under the assumption that the chains can be modeled as two overlapping Gaussian charge profiles. The analytical calculations are compared with measurements from Molecular Dynamics simulations. Good quantitative agreement is found for charging fractions below 10%, where the chains assume coil-like configurations, whereas deviations develop for charge fraction of 20%, in which case a conformational transition of the chain towards a rodlike configuration starts to take place.Comment: 38 pages, 12 figures, 2 tables. Revised version of the manuscript. Selected for publication in the V\irtual Journal of Biological Physics Research, issue of 1 september, 200