Non-linear optical spectra of excitons in polydiacetylene

Abstract Adding long-range Coulomb interactions to the Su-Schrieffer-Heeger model makes it possible to investigate excitonic states in conjugated polymers. Various characteristic features due to these states as well as due to the electron-hole continuum can be found in the calculated non-linear optical susceptibilities. In particular the electroabsorption spectrum and the third harmonic generation intensity and its dependence on the system size are examined. Using only moderate interaction strength, various experiments in polydiacetylene can be interpreted in a consistent way.