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000450054 245__ $$aTime-resolving the UV-initiated photodissociation dynamics of OCS
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000450054 520__ $$aWe present a time-resolved study of the photodissociation dynamics of OCS after UV- photoexcitation at λ = 237 nm. OCS molecules (X 1Σ+) were primarily excited to the 1 1A′′ and the 2 1A′ Renner-Teller components of the 1Σ− and 1∆ states. Dissociation into CO and S fragments was observed through time-delayed strong-field ionisation and imaging of the kinetic energy of the resulting CO+ and S+ fragments by intense 790 nm laser pulses. Surprisingly, fast oscillations with a period of ∼100 fs were observed in the S+ channel of the UV dissociation. Based on wavepacket-dynamics simulations coupled with a simple electrostatic-interaction model, these oscillations do not correspond to the known highly-excited rotational motion of the leaving CO(X 1Σ+, J ≫ 0) fragments, which has a timescale of ∼140 fs. Instead, we suggest to assign the observed oscillations to the excitation of vibrational wavepackets in the 2 3A′′ or 2 1A′′ states of the molecule that predissociate to form S(3PJ ) photoproducts.
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