Effects of Structural Fluctuations on Two-Photon Absorption Activity of Interacting Dipolar Chromophores

Abstract

One- and two-photon absorption properties of organic chromophores consisting of interacting dipolar branches have been studied using density functional response theory in combination with molecular dynamics simulation. Effects of dipole interaction on optical absorptions have been examined. The importance of solvent effects on optical properties of charge-transfer states is explored by means of polarizable continuum model. It is found that for the interacting dipolar molecule with flexible conformations in solutions, the structural fluctuations can result in new spectral features or significant broadening of one-photon absorption spectrum. Our study highlights again the usefulness of the combined quantum chemical and molecular dynamics approach for modeling two-photon absorption materials in solutions.