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.
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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-pp.ucl.ac.uk/id/eprint/10099245 |
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