Elongated push–pull diphenylpolyenes for nonlinear optics: molecular engineering of quadratic and cubic optical nonlinearities via tuning of intramolecular charge transfer

Abstract Push–pull polyenes are of particular interest for nonlinear optics (NLO) as well as model compounds for long-distance intramolecular charge transfer (ICT). In order to tune the ICT phenomenon and control the linear and nonlinear optical properties, we have synthesized and investigated several series of soluble push–pull diphenylpolyenes of increasing length and having various donor (D) and acceptor (A) end groups. Their linear and NLO properties have been studied by performing electro-optical absorption measurements (EOAM) and third-harmonic generation (THG) experiments in solution. Each push–pull molecule exhibits an intense ICT absorption band in the visible characterized by an i…