Molecular Dynamics Simulations of Electric Field Poled Poly(methyl methacrylate) Doped with Tricyanopyrroline Chromophores

Nonlinear optical polymer-based materials are promising candidates for future high-bandwidth data processing and other optically driven applications. This class of materials consists of noncentrosymmetrically aligned electro-optic (EO) active chromophores embedded in a polymer matrix. However, there are no experimental measurement methods available to directly investigate the molecular orientation of individual chromophore molecules in the polymer matrix. Therefore, a reliable simulation protocol was developed to fill this gap. This study extends previous work in the context of larger atomistic polymer models and a contemporary chromophore molecule. In contrast to earlier approaches, a quantum mechanical continuum solvation method is introduced to account for local field effects. The experimentally accessible EO tensor element r₃₃ is calculated and contextualized with other studies; good agreement with experimental values is demonstrated. We provide a comprehensive molecular simulation protocol for the design, development, and analysis of novel materials.