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Identification and Role of Two-Photon Excited States in a<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mi>π</mml:mi></mml:math>-Conjugated Polymer

Brian LawrenceCenter for Research in Electro-Optics and Lasers, University of Central Florida, 12424 Research Parkway, Orlando, Florida 32826William E. TorruellasCenter for Research in Electro-Optics and Lasers, University of Central Florida, 12424 Research Parkway, Orlando, Florida 32826M. ChaCenter for Research in Electro-Optics and Lasers, University of Central Florida, 12424 Research Parkway, Orlando, Florida 32826M.L. SundheimerCenter for Research in Electro-Optics and Lasers, University of Central Florida, 12424 Research Parkway, Orlando, Florida 32826G. I. StegemanCenter for Research in Electro-Optics and Lasers, University of Central Florida, 12424 Research Parkway, Orlando, Florida 32826Jeffrey S. MethCenter for Research in Electro-Optics and Lasers, University of Central Florida, 12424 Research Parkway, Orlando, Florida 32826S. EtemadCenter for Research in Electro-Optics and Lasers, University of Central Florida, 12424 Research Parkway, Orlando, Florida 32826Gregory L. BakerCenter for Research in Electro-Optics and Lasers, University of Central Florida, 12424 Research Parkway, Orlando, Florida 32826
1994en
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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 ${n}_{2}$ is also reported.

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