Abstract

Third-harmonic generation measurements have been made for the first time on oriented films of halogen-bridged mixed-valence platinum complexes for the pump wavelength region from 0.6 to 1.0 μm. The ‖χ(3)(−3ω;ω,ω,ω)‖ spectra obtained by the Maker’s fringe method show a distinct peak at about 1.8 eV with the peak value of about 4×10−11 esu. From comparison with the electroabsorption data, this peak has been identified with the two-photon resonance peak with the forbidden exciton in the Pt-halogen chains. One-dimensional exciton states in this compound take an important role in the third-order optical nonlinearity, similar to the case in conjugated polymers.

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