A high performing electro-optic ( EO) chromophore with covalently attached coumarin-based pendant groups exhibits intermolecular correlation of coumarin units through molecular dynamics ( MD) simulations. Unique, orthogonal molecular orientations of the chromophore and coumarin units are also evident when investigated optically. Such molecular orientation translates to reduced lattice dimensionality of the bulk C1 soft matter material system, leading to increased acentric order and EO activity. Results are corroborated by nanorheological experimental methods.