Extending Graph-based Lattice Kinetic Monte Carlo Simulations to Polymer Transformations

Multiscale simulations offer a way to understand how polymer transformations proceed under realistic conditions, however existing workflows rely on empirically tuned parameters. The MUltiscale SImulation frameworK (MUSIK) integrates conformer analysis, density functional theory and high-level coupled-cluster energetics, and graph-based lattice kinetic Monte Carlo (kMC) to generate chemically accurate, spatially and temporally resolved kinetic models for polymer transformations without parameter fitting. The present work introduces MUSIK as a reproducible workflow and provides a step-by-step tutorial that shows how to construct, run, and analyze a lattice kMC model for base-assisted dehydrochlorination of polyvinyl chloride (PVC), supported by post-processing scripts that automate kMC trajectory analysis and polymer-structure reconstruction. Tutorial results demonstrate how MUSIK links atomic energetics and local structure to macroscopic kinetics and structural evolution and reproduces key experimental observations for PVC dehydrochlorination. MUSIK is generalizable to arbitrary polymer chemistries and can provide practical recommendations for polymer recycling, upcycling, and materials design to address plastic-waste challenge.