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Full observation of ultrafast cascaded radiationless transitions from S₂(ππ*) state of pyrazine using vacuum ultraviolet photoelectron imaging

Horio, T; Spesyvtsev, R; Nagashima, K; Ingle, RA; Suzuki, Y-I; Suzuki, T; (2016) Full observation of ultrafast cascaded radiationless transitions from S₂(ππ*) state of pyrazine using vacuum ultraviolet photoelectron imaging. The Journal of Chemical Physics , 145 (4) , Article 044306. 10.1063/1.4955296. Green open access

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Abstract

A photoexcited molecule undergoes multiple deactivation and reaction processes simultaneously or sequentially, which have been observed by combinations of various experimental methods. However, a single experimental method that enables complete observation of the photo-induced dynamics would be of great assistance for such studies. Here we report a full observation of cascaded electronic dephasing from S_{2}(ππ*)in pyrazine (C_{4}N_{2}H_{4}) by time-resolved photoelectron imaging (TRPEI) using 9.3-eV vacuum ultraviolet pulses with a sub-20 fs time duration. While we previously demonstrated a real-time observation of the ultrafast S_{2}(ππ*) → S_{1}(nπ*)internal conversion in pyrazine using TRPEI with UV pulses, this study presents a complete observation of the dynamics including radiationless transitions from S_{1} to S_{0} (internal conversion) and T_{1}(nπ*) (intersystem crossing). Also discussed are the role of {1}^A_{u}(nπ*) in the internal conversion and the configuration interaction of the S_{2}(ππ*) electronic wave function.

Type: Article
Title: Full observation of ultrafast cascaded radiationless transitions from S₂(ππ*) state of pyrazine using vacuum ultraviolet photoelectron imaging
Open access status: An open access version is available from UCL Discovery
DOI: 10.1063/1.4955296
Publisher version: https://doi.org/10.1063/1.4955296
Language: English
Additional information: This version is the version of record. For information on re-use, please refer to the publisher's terms and conditions.
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/10099245
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