Coarse-grained Monte Carlo/molecular dynamic calculations are employed to explore the effect of various of
intermolecular electrostatic interactions upon chromophore order, lattice dimensionality, and viscoelasticity in
electrically-poled organic second order nonlinear optical materials. The following classes of organic macromolecular materials are considered: (1) Chromophore-polymer composites, (2) chromophores covalently incorporated into polymers and dendrimers, (3) chromophores incorporating additional dipolar or quadrupolar interactions that enhance poling efficiency, and (4) binary chromophore materials. For chromophore-polymer composites, the competition of chromophore-chromophore dipolar interactions and nuclear repulsive (steric) interactions define poling-induced acentric order. For covalently incorporated chromophores, covalent bond potentials also influence poling-induced order. These first two classes of materials basically behave as Langevin (3-D) lattice materials. Dipolar (e.g., coumarin) and quadrupolar (arene-perfluoroarene) interactions act to influence lattice dimensionality and thus enhance poling efficiency (the ratio of electro-optic activity to electric poling field strength). The long-range molecular cooperativity associated with these interactions influences viscoelastic properties critical to material processing and integration into silicon photonic, plasmonic, and metamaterial devices. The interaction between different chromophore species in binary chromophore materials also enhances poling efficiency. Polarized laser radiation applied to certain binary chromophore materials can also be used to enhance poling efficiency through control of lattice dimensionality. Poling efficiency approaching 5 (nm/V)2 has been achieved for these latter two classes of materials. Improvement in poling efficiency and control of material viscosity is particular important for integration of organic materials into complex device structures.