Abstract
The frequency dependence of the third harmonic generation in trans-polyacetylene is quantitatively interpreted by considering the bands of finite chain and the damping of excitation. Our theory shows that there are two distinct peaks in the spectrum of the third harmonic generation. The first one around 0.6 eV comes from the three-photon resonant transition between the edges of the valence band and conduction band; the second one around 0.9 eV is produced by the two-photon interband transition. The excitation-dependent damping is essential to determine the position of the second peak. The theoretical results agree well with the experimental data.
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