Combined coarse-grained molecular dynamics and finite-element study of light-activated deformation of photoresponsive polymers

Abstract

The azobenzene-containing crosslinked liquid crystalline polymer is a potential candidate for a stimuli-responsive soft robot, as it provides contactless actuation without the implementation of any separate component. For facilitating practical applications of this novel material, complicated and predefined motions have been realized by tailoring the chemical structure of the polymer network. However, conventional multiscale mechanical analysis, which utilizes the all-atom molecular dynamics to represent a microscopic model, is unsuitable for handling diverse material design parameters due to excessive computational costs. Hence, a multiscale optomechanical simulation framework, which combines the coarse-grained molecular dynamics (CG MD) and the finite-element (FE) method, is developed in this study. The CG MD simulation satisfactorily reproduces the light-induced phase transition and photosoftening effect on the mechanical properties. In particular, using the mesoscale analysis, the presented methodology can treat diverse morphology parameters (liquid crystal phase, spacer length, and crosslinking density) to observe the associated photodeformations. The photostrain and elastic modulus profiles in terms of photoisomerization ratio are implemented into the continuum-scale governing equation, which is based on the neoclassical elasticity theory. To efficiently reflect the light-induced large rotations of liquid crystal mesogens and the corresponding geometric nonlinearity, a corotational formulation is employed in the FE shell model. We examine the mesostructural-morphology-dependent photobending deformations of the nematic and smectic photoresponsive polymers (PRPs). In addition, the mesoscopic-texture-mediated unique 3D deformations are investigated by modeling the topological defects. This study offers insight into the engineering of PRP materials for designing the mechanical motions of smart actuators.