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Mechanochemical Activation of Spiropyran in PMMA - A Hybrid Quantum Chemical/Atomistic/Coarse-Grained Approach
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DOI：10.1002/mame.202500471.png)
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Abstract
En 中文
Embedding mechanophores into polymer matrices to activate mechanochemical reactions has been extensively employed to realize diverse functional applications. Spiropyran (SP) is a widely used mechanophore that undergoes force-induced isomerization into its activated merocyanine (MC) form, accompanied by a color change. To accurately simulate the SP-MC isomerization process under tension, the present work introduces a large-scale hybrid coarse-grained/atomistic (CG/AA) model in which poly(methyl metacrylate) (PMMA) monomers are represented by individual beads, while SP remains fully described at the AA level. We used force field parameters derived from quantum chemical (QC) data, employing the fully atomistic framework previously developed by our group. This approach enabled deformation simulations of significantly larger systems than possible with a pure AA force field, at reduced computational cost, thereby providing novel insights into force transduction and mechanophore activation. The simulations demonstrated the dependence of the activation rate on system size and yielded realistic onset strains, comparable with experimental observations. Furthermore, a parabolic stress distribution was observed along individual PMMA chains, resulting in preferential SP activation near chain centers. Non-specific chain scission events occurred far less frequently than SP activations. The developed hybrid model offers a powerful framework for investigating more complex mechanophore-doped polymer networks.
Keywords:
activation rate
defects
mechanophore activation and mechanochromism
onset strain
spiropyran-doped hybrid CG/AA model
stress distribution along chains
tensile deformation simulation
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