Nonlinear Optical Properties of Correlated Chromophores in Organic Mesoscopic Superstructures

A new design strategy for enhanced nonlinear optical properties, based on a simple vector model and situated at the mesoscopic level, between the microscopic molecular level and the macroscopic bulk, is explained and exemplified by a number of organic superstructures. The second-order nonlinear optical properties of the structures are analyzed in terms of the corresponding properties of the individual monomeric chromophores that constitute the structure. The chromophores can be considered as electronically independent with a high symmetry. A simple vector model can then account for the large secondorder nonlinear optical polarizability of the mesoscopic superstructure. Another important advantage that is clear from the vector analysis is the improved chromophore alignment, owing to the enlarged mesoscopic dipole moment.