Quantitative Prediction of Two-Photon Absorption Cross Section Based on Linear Spectroscopic Properties

We study two-photon absorption (2PA) spectra in a broad class of organic dye molecules, such as substituted diphenylaminostilbenes, push−pull porphyrins, and carbazol-substituted stilbenes. We show, for the first time, that the 2PA cross section in the lowest-energy dipole-allowed transition may be predicted with better than 50% absolute accuracy based solely on the molecular parameters obtained from linear spectroscopic measurements.