Figueira Nunes, Joao Pedro;
Ibele, Lea Maria;
Pathak, Shashank;
Attar, Andrew R;
Bhattacharyya, Surjendu;
Boll, Rebecca;
Borne, Kurtis;
... Curchod, Basile FE; + view all
(2024)
Monitoring the Evolution of Relative Product Populations at Early Times during a Photochemical Reaction.
Journal of the American Chemical Society
10.1021/jacs.3c13046.
(In press).
Preview |
Text
figueira-nunes-et-al-2024-monitoring-the-evolution-of-relative-product-populations-at-early-times-during-a.pdf - Published Version Download (4MB) | Preview |
Abstract
Identifying multiple rival reaction products and transient species formed during ultrafast photochemical reactions and determining their time-evolving relative populations are key steps toward understanding and predicting photochemical outcomes. Yet, most contemporary ultrafast studies struggle with clearly identifying and quantifying competing molecular structures/species among the emerging reaction products. Here, we show that mega-electronvolt ultrafast electron diffraction in combination with ab initio molecular dynamics calculations offer a powerful route to determining time-resolved populations of the various isomeric products formed after UV (266 nm) excitation of the five-membered heterocyclic molecule 2(5H)-thiophenone. This strategy provides experimental validation of the predicted high (∼50%) yield of an episulfide isomer containing a strained three-membered ring within ∼1 ps of photoexcitation and highlights the rapidity of interconversion between the rival highly vibrationally excited photoproducts in their ground electronic state.
| Type: | Article |
|---|---|
| Title: | Monitoring the Evolution of Relative Product Populations at Early Times during a Photochemical Reaction |
| Location: | United States |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1021/jacs.3c13046 |
| Publisher version: | http://dx.doi.org/10.1021/jacs.3c13046 |
| Language: | English |
| Additional information: | © 2024 The Authors. Published by American Chemical Society. This publication is licensed under CC-BY 4.0. You are free to share (copy and redistribute) this article in any medium or format and to adapt (remix, transform, and build upon) the material for any purpose, even commercially within the parameters below: cc licence Creative Commons (CC): This is a Creative Commons license. ny licence Attribution (BY): Credit must be given to the creator. |
| Keywords: | Computational chemistry, Diffraction, Molecular structure, Molecules, Photoexcitation |
| 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/10186903 |
Archive Staff Only
 |
View Item |
