Abstract
Doppler-free two-photon electronic spectra of a large polyatomic molecule are recorded for the first time with pulsed laser radiation of near Fourier-transform limited bandwidth (Δ v∼100 MHz). The resolution obtained is sufficient to resolve individual rotational lines. Due to the high density of these rotational transitions a strong Doppler-broadened background is observed, which is, however, subtantially reduced by suitable choice of photon polarizations. Different vibronic bands of benzene (C 6H 6) are investigated and very accurate rotational constants are found.
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