Modeling Targeted Mechanochemistry in Polymeric Solids

Embedding mechanophores into polymeric solids enables the design of materials that respond to mechanical stimuli, with applications in sensing, self-healing, and adaptive systems. This review summarizes modeling approaches for mechanophores in polymer solids across multiple length scales, from nanoscale quantum chemical models and mesoscale reactive molecular dynamics to macroscale continuum frameworks. We also discuss theoretical foundations such as force-modified potential energy surfaces. We then compare computational strategies to experimental insights, highlighting key findings, ranging from the roles of mechanophore geometry, chemical substituents, network architecture, and physical cross-linking in force transduction and activation. Persistent challenges in the field include capturing multiscale dynamics, local environmental effects, and heterogeneity. Advancing predictive models will accelerate mechanophore discovery and enable rational design of mechanoresponsive polymeric solids.