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We have observed second-harmonic generation (SHG) and third-harmonic generation (THG) spectra in polydiacetylene (PDA), poly[5,7-dodecadiyne-1,12-diyl-bis-ethylurethane], thin films. According to linear absorption and THG spectra in PDA, two dipole-allowed states, the lowest B u exciton and the band edge, exist around 2.0 eV and 2.6 eV, respectively. Therefore, a resonant peak appearing around...
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