Abstract
The vibrationless S 1( 1B 3u) state of pyrazine has been investigated by time-resolved spectroscopy with Fourier transform-limited nanosecond laser pulses. The appearance of biexponential fluorescence decays was found to depend strongly on the laser pulse energy between 1.5 and 320 μJ, corresponding to estimated spectral intensities of 11 and 2200 W/MHz cm 2, respectively. The behaviour observed at the lowest pulse enegies is discussed in the light of explanations given for the fast emission component in the literature, and agrees best with near resonance Raman scattering/resonance fluorescence of an intermediate level structure. Contradictions in the dynamics apparent in published data are resolved if saturation effects are taken into account.
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