Monitoring the evolution of relative product populations at early times during a photochemical reaction

  • João Pedro Figueira Nunes (Creator)
  • Matthias Hoffmann (Creator)
  • Andrew Attar (Creator)
  • Xiaozhe Shen (Creator)
  • Duan Luo (Creator)
  • Sri Bhavya Muvva (Creator)
  • Artem Rudenko (Creator)
  • Anbu Venkatachalam (Creator)
  • Rebecca Boll (Creator)
  • Xijie Wang (Creator)
  • Yanwei Xiong (Creator)
  • Sajib Kumar Saha (Creator)
  • Kurtis Borne (Creator)
  • Surjendu Bhattacharyya (Creator)
  • Kyle Wilkin (Creator)
  • Christopher Hansen (Creator)
  • Jie Yang (Creator)
  • Ruaridh Forbes (Creator)
  • Lea M. Ibele (Creator)
  • Arnaud Rouzée (Creator)
  • Martin Centurion (Creator)
  • Ming-Fu Lin (Creator)
  • Nathan Goff (Creator)
  • Stephen Weathersby (Creator)
  • Benjamin Erk (Creator)
  • Thomas Wolf (Creator)
  • Shashank Pathak (Creator)
  • Matthew Ware (Creator)
  • Alex Reid (Creator)
  • Rebecca Ingle (Creator)
  • Michael N R Ashfold (Creator)
  • David M Holland (Creator)
  • Daniel Rolles (Creator)
  • Basile F E Curchod (Creator)

Dataset

Description

Identifying multiple rival reaction products and transient species formed during ultrafast photochemical reactions and determining their time-evolving relative populations are key steps towards understanding and predicting photochemical outcomes. Yet, most contemporary ultrafast studies struggle with clearly identifying and quantifying competing molecular structures/species amongst the emerging reaction products. Here, we show that mega-electronvolt ultrafast electron diffraction in combination with ab initio molecular dynamics calculations offers a unique route to determine time-resolved populations of the various isomeric products formed after UV (266 nm) excitation of the five-membered heterocyclic molecule thiophenone. This strategy reveals an unexpectedly high (~50%) yield of an episulfide isomer containing a strained 3-membered ring within ~1 ps at early times and rapid interconversions between the rival photoproducts.
Date made available3 May 2023
PublisherDryad

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