Identification and Role of Two-Photon Excited States in aπ-Conjugated Polymer

Abstract
We have measured the full two-photon absorption (TPA) spectrum in the transparency range of single-crystal polydiacetylene paratoluene-sulfonate (PTS) using z scan. The spectrum consists of three well-defined two-photon excited states superimposed on a continuum of even-parity states. Comparison of the TPA and the one-photon absorption spectra identifies a two-photon accessible state as the lowest excited state of PTS. The accompanying dispersion in the intensity-dependent refractive index coefficient n2 is also reported.