Large Quadratic Hyperpolarizabilities with Donor–Acceptor Polyenes Exhibiting Optimum Bond Length Alternation: Correlation Between Structure and Hyperpolarizability

Donor-acceptor polyenes of various lengths, and that combine aro- matic electron-donating moieties with powerful heterocyclic electron-withdraw- ing terminal groups, have been synthe- sized and characterized as efficient non- linear optical (NLO) chromophores. Their linear and nonlinear optical proper- ties have been investigated, and variations in these properties have been related to ground-state polarization (dipole p) and structure. In particular, unprecedented quadratic hyperpolarizabilities (p) have been achieved (up to p(0) =I500 x 10-30esu) by reduction of the bond- length alternation (BLA) in the polyenic chain. In each series of homologous com-