Abma, Grite L;
Parkes, Michael A;
Razmus, Weronika O;
Zhang, Yu;
Wyatt, Adam S;
Springate, Emma;
Chapman, Richard T;
... Minns, Russell S; + view all
(2024)
Direct Observation of a Roaming Intermediate and Its Dynamics.
Journal of the American Chemical Society
, 146
(18)
12595 -12600.
10.1021/jacs.4c01543.
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Abstract
Chemical reactions are often characterized by their transition state, which defines the critical geometry the molecule must pass through to move from reactants to products. Roaming provides an alternative picture, where in a dissociation reaction, the bond breaking is frustrated and a loosely bound intermediate is formed. Following bond breaking, the two partners are seen to roam around each other at distances of several Ångstroms, forming a loosely bound, and structurally ill-defined, intermediate that can subsequently lead to reactive or unreactive collisions. Here, we present a direct and time-resolved experimental measurement of roaming. By measuring the photoelectron spectrum of UV-excited acetaldehyde with a femtosecond extreme ultraviolet pulse, we captured spectral signatures of all of the key reactive structures, including that of the roaming intermediate. This provided a direct experimental measurement of the roaming process and allowed us to identify the time scales by which the roaming intermediate is formed and removed and the electronic potential surfaces upon which roaming proceeds.
| Type: | Article |
|---|---|
| Title: | Direct Observation of a Roaming Intermediate and Its Dynamics |
| Location: | United States |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1021/jacs.4c01543 |
| Publisher version: | http://dx.doi.org/10.1021/jacs.4c01543 |
| Language: | English |
| Additional information: | Copyright © 2024 The Authors. Published by American Chemical Society. This publication is licensed under CC-BY 4.0, (https://creativecommons.org/licenses/by/4.0/). |
| 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/10191908 |
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