Theoretical study on the near-resonant second hyperpolarizability (γ) of a dendritic molecular aggregate: the spatial contribution of intermolecular-interaction and relaxation to γ

Second hyperpolarizability (γ) of a dendritic molecular aggregate (D25) in the resonant region is calculated using a two-exciton coupled-dipole model. Using a visualization method of exciton generation to y, there is found to be a significant difference in the spatial contribution between intermolecular-interaction and relaxation effects on γ, which is dramatically changed compared to the case of the dendritic aggregate without intermolecular-interaction.