Abstract
Third-order nonlinear-optical susceptibility spectra \ensuremath{\Vert}${\mathrm{\ensuremath{\chi}}}^{(3)}$(-3\ensuremath{\omega};\ensuremath{\omega},\ensuremath{\omega},\ensuremath{\omega})\ensuremath{\Vert} have been obtained for poly(dihexylsilane) (PDHS) and poly(dibutylsilane) (PDBS) films by third-harmonic generation (THG) measurements for a fundamental photon energy region from 1.90 to 2.15 eV, which covers the two-photon absorption (TPA) for PDHS but not for PDBS. The \ensuremath{\Vert}${\mathrm{\ensuremath{\chi}}}^{(3)}$\ensuremath{\Vert} spectrum for PDHS shows a prominent peak at about 2.08 eV with a maximum value of about 2.3\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}12}$ esu, while there is no enhancement effect in PDBS in the same fundamental photon energy region. These results provide direct evidence for the two-photon-resonant THG process in polysilanes due to the one-photon-forbidden $^{1}$${\mathit{A}}_{\mathit{g}}$ exciton detected by TPA and electroabsorption measurements.
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