Predicting experimental results for polyethylene by computer simulation

Abstract

This feature article reviews several aspects of computational approaches to polyethylene melt and solid state properties in relation to existing experimental results. Based on 40 years of experience in the field, we offer a personal view of how computer simulations are helping to understand the physics of polyethylene as a model polymer. The first issue discussed is the molten state of polyethylene, including static and dynamic properties and entanglement features along with their impacts on rheological behaviour. We then examine the glass transition, crystallization process and solid state structure, including the interlamellar region. This is followed by brief descriptions of the latest advances in simulating mechanical properties and of the various methodologies used to simulate the physics of polyethylene. Throughout the manuscript, references are made to our own work and also to studies by many other authors that have nicely contributed to developments in simulating the physics of polyethylene in close agreement with experimental results.

All-atomic and coarse-grained molecular dynamics investigation of deformation in semi-crystalline lamellar polyethylene

“…This is in contrast to cavity formation, which is seen in the all-atomic modelling and is closely associated with the lamellar separation mode [50]. Similar types of inconsistencies have been observed when modelling rheological properties in liquid polymers, see for instance [61][62][63][64], and it implies that time-scaling is necessary to associate the observed mechanisms with experimental or all-atomic results. This behaviour suggests that the potentials have intrinsic rates or activation times for competing mechanisms, which is in line with previously reported results that have demonstrated a clear strain rate dependence [26].…”

Toward realistic computer modeling of paraffin-based composite materials: critical assessment of atomic-scale models of paraffins

“…For the sake of consistency, the Nosé-Hoover thermostat was employed for these three systems. 44,45 The time constant s T was set to 1 ps with the exceptions of OPLS-AA/L-OPLS-AA systems, for which s T was 0.1 ps.…”

“…A good overview of performance of united-atom force elds in simulations of polyethylene can be found in a recent review paper. 45 To meet a lack of a systematic comparison between alkane-specic and general-purpose force elds, we selected 10 most popular force elds and assessed carefully their performance in computer simulations of paraffins.…”

Atomistic hybrid particle‐field molecular dynamics combined with slip‐springs: Restoring entangled dynamics to simulations of polymer melts

“…As a reference, the experimental entanglement length of PE melts is around N = 85. [41] The study of entangled PE requires long simulation times to show the features of entangled dynamics. The choice of united-atom model of PE reduces the computing expense.…”