Gespeichert in:
| Hauptverfasser: | , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , |
|---|---|
| Format: | Preprint |
| Veröffentlicht: |
2023
|
| Schlagworte: | |
| Online-Zugang: | https://arxiv.org/abs/2311.12482 |
| Tags: |
Tag hinzufügen
Keine Tags, Fügen Sie den ersten Tag hinzu!
|
| _version_ | 1866914946945646592 |
|---|---|
| author | Nunes, Joao Pedro Figueira Ibele, Lea Maria Pathak, Shashank Attar, Andrew R. Bhattacharyya, Surjendu Boll, Rebecca Borne, Kurtis Centurion, Martin Erk, Benjamin Lin, Ming-Fu Forbes, Ruaridh J. G. Goff, Nate Hansen, Christopher S. Hoffmann, Matthias Holland, David M. P. Ingle, Rebecca A. Luo, Duan Muvva, Sri Bhavya Reid, Alex Rouzée, Arnaud Rudenko, Artem Saha, Sajib Kumar Shen, Xiaozhe Venkatachalam, Anbu Selvam Wang, Xijie Ware, Matt R. Weathersby, Stephen P. Wilkin, Kyle Wolf, Thomas J. A. Xiong, Yanwei Yang, Jie Ashfold, Michael N. R. Rolles, Daniel Curchod, Basile F. E. |
| author_facet | Nunes, Joao Pedro Figueira Ibele, Lea Maria Pathak, Shashank Attar, Andrew R. Bhattacharyya, Surjendu Boll, Rebecca Borne, Kurtis Centurion, Martin Erk, Benjamin Lin, Ming-Fu Forbes, Ruaridh J. G. Goff, Nate Hansen, Christopher S. Hoffmann, Matthias Holland, David M. P. Ingle, Rebecca A. Luo, Duan Muvva, Sri Bhavya Reid, Alex Rouzée, Arnaud Rudenko, Artem Saha, Sajib Kumar Shen, Xiaozhe Venkatachalam, Anbu Selvam Wang, Xijie Ware, Matt R. Weathersby, Stephen P. Wilkin, Kyle Wolf, Thomas J. A. Xiong, Yanwei Yang, Jie Ashfold, Michael N. R. Rolles, Daniel Curchod, Basile F. E. |
| contents | 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 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 3-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. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2311_12482 |
| institution | arXiv |
| publishDate | 2023 |
| record_format | arxiv |
| spellingShingle | Monitoring the evolution of relative product populations at early times during a photochemical reaction Nunes, Joao Pedro Figueira Ibele, Lea Maria Pathak, Shashank Attar, Andrew R. Bhattacharyya, Surjendu Boll, Rebecca Borne, Kurtis Centurion, Martin Erk, Benjamin Lin, Ming-Fu Forbes, Ruaridh J. G. Goff, Nate Hansen, Christopher S. Hoffmann, Matthias Holland, David M. P. Ingle, Rebecca A. Luo, Duan Muvva, Sri Bhavya Reid, Alex Rouzée, Arnaud Rudenko, Artem Saha, Sajib Kumar Shen, Xiaozhe Venkatachalam, Anbu Selvam Wang, Xijie Ware, Matt R. Weathersby, Stephen P. Wilkin, Kyle Wolf, Thomas J. A. Xiong, Yanwei Yang, Jie Ashfold, Michael N. R. Rolles, Daniel Curchod, Basile F. E. Chemical Physics 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 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 3-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. |
| title | Monitoring the evolution of relative product populations at early times during a photochemical reaction |
| topic | Chemical Physics |
| url | https://arxiv.org/abs/2311.12482 |