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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.
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Lawrence et al. (1994) studied this question.
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