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Volume 228, 2021

Time-resolving the UV-initiated photodissociation dynamics of OCS

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Abstract

We present a time-resolved study of the photodissociation dynamics of OCS after UV-photoexcitation at λ = 237 nm. OCS molecules (X1Σ+) were primarily excited to the 11A′′ and the 21A′ Renner–Teller components of the 1Σ and 1Δ 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(X1Σ+, 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 23A′′ or 21A′′ states of the molecule that predissociate to form S(3PJ) photoproducts.

Graphical abstract: Time-resolving the UV-initiated photodissociation dynamics of OCS

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Supplementary files

Article information


Submitted
15 Oct 2020
Accepted
27 Oct 2020
First published
29 Oct 2020

Faraday Discuss., 2021,228, 413-431
Article type
Paper

Time-resolving the UV-initiated photodissociation dynamics of OCS

E. T. Karamatskos, S. Yarlagadda, S. Patchkovskii, M. J. J. Vrakking, R. Welsch, J. Küpper and A. Rouzée, Faraday Discuss., 2021, 228, 413 DOI: 10.1039/D0FD00119H

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