Abstract
Results of optical second-harmonic generation and wave-dispersed third-harmonic generation measurements in C 60 thin films are reported and discussed. In third-harmonic generation measurements two strong resonances in cubic susceptibility χ (3)(−3ω; ω, ω, ω) are observed. The first one occurring at 1.3 μm fundamental wavelength is interpreted in terms of a three-photon resonance with vibronic components of gerade states made partially allowed by vibronic mixing with the higher T 1u state. The second resonance at 1.064 μm is interpreted as a three-photon resonance with the T 1u state. The measured resonant values of χ (3)(−3ω; ω, ω, ω) are 6.1 × 10 −11 and 8.2 × 10 −11 e.s.u. at 1.3 and 1.064 μm, respectively. The second-harmonic generation measurements performed at 1.064 μm on native thin films lead to a significant second-order susceptibility d pp(−2 ω; ω, ω) = 3.8 × 10 −9 e.s.u. (1.6 pm/V).
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