Coarse-Grained Artificial Intelligence for Design of Brush Networks

The ability to synthesize elastomeric materials with programmable mechanical properties is vital for advanced soft matter applications. Due to the inherent complexity of hierarchical structure-property correlations in brush-like polymer networks, the application of conventional theory-based, so-called Human Intelligence (HI) approaches becomes increasingly difficult. Herein we developed a design strategy based on synergistic combination of HI and AI tools which allows precise encoding of mechanical properties with three architectural parameters: degrees of polymerization (DP) of network strands, n, side chains, n_sc, backbone spacers between side chains, n_g. Implementing a multilayer feedforward artificial neural network (ANN), we took advantage of model-predicted structure-property cross-correlations between coarse-grained system code including chemistry specific characteristics S = [l, v, b] defined by monomer projection length l and excluded volume v, Kuhn length b of bare backbone and side chains, and architecture A = [n_sc, n_g, n] of polymer networks and their equilibrium mechanical properties P = [G, β] including the structural shear modulus G and firmness parameter β. The ANN was trained by minimizing the mean-square error with Bayesian regularization to avoid overfitting using a data set of experimental stress-deformation curves of networks with brush-like strands of poly(n-butyl acrylate), poly(isobutylene), and poly(dimethylsiloxane) having structural modulus G < 50 kPa and 0.01 ≤ β ≤ 0.3. The trained ANN predicts network mechanical properties with 95% confidence. The developed ANN was implemented for synthesis of model networks with identical mechanical properties but different chemistries of network strands.