Jamming and crystallization in athermal polymer packings

Dense packings of chains of hard spheres possess characteristic features that do not have a counterpart in corresponding packings of monomeric spheres especially near the maximally random jammed (MRJ) state. From the modelling perspective the additional requirement that spheres keep their connectivity while maximizing the occupied volume fraction imposes severe constraints on generation algorithms of dense chain configurations. The extremely sluggish dynamics imposed by the uncrossability of chains precludes the use of deterministic or stochastic dynamics to generate all but dilute polymer packings. As a viable alternative, especially tailored chain-connectivity-altering Monte Carlo (MC) algorithms have been developed that bypass this kinetic hindrance and have actually been able to produce packings of hard-sphere chains in a volume fraction range spanning from infinite dilution up to the MRJ state. Such very dense athermal polymer packings share a number of structural features with packings of monomeric ...