Perspective on a challenge: predicting the photochemistry of cyclobutanone
Fuente:
arXiv
Saved in:
| Main Authors: | , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , |
|---|---|
| Format: | Preprint |
| Published: |
2026
|
| Subjects: | |
| Online Access: | |
| Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
| _version_ | 1866917412753899520 |
|---|---|
| author | Janoš, Jiří List, Nanna Holmgaard Orr-Ewing, Andrew J. Suchan, Jiří Barbatti, Mario Bennett, Olivia Brady, Marcus Carmona-García, Javier Crespo-Otero, Rachel Eng, Julien Fajen, O. Jonathan Garavelli, Marco Gómez, Sandra Green, Alice E. Hernández, Federico J. Hollas, Daniel Hutton, Lewis Ibele, Lea M. Kirrander, Adam Lan, Zhenggang Lassmann, Yorick Lawrence, Joseph E. Levine, Benjamin G. Makhov, Dmitry V. Mannouch, Jonathan R. Miao, Xincheng Mitrić, Roland Parker, Shane M. Penfold, Thomas J. Peng, Jiawei Richardson, Jeremy O. Shalashilin, Dmitrii Slavíček, Petr Spinlove, K. Eryn Vindel-Zandbergen, Patricia Agostini, Federica Bonella, Sara Martínez, Todd J. Worth, Graham A. Curchod, Basile F. E. |
| author_facet | Janoš, Jiří List, Nanna Holmgaard Orr-Ewing, Andrew J. Suchan, Jiří Barbatti, Mario Bennett, Olivia Brady, Marcus Carmona-García, Javier Crespo-Otero, Rachel Eng, Julien Fajen, O. Jonathan Garavelli, Marco Gómez, Sandra Green, Alice E. Hernández, Federico J. Hollas, Daniel Hutton, Lewis Ibele, Lea M. Kirrander, Adam Lan, Zhenggang Lassmann, Yorick Lawrence, Joseph E. Levine, Benjamin G. Makhov, Dmitry V. Mannouch, Jonathan R. Miao, Xincheng Mitrić, Roland Parker, Shane M. Penfold, Thomas J. Peng, Jiawei Richardson, Jeremy O. Shalashilin, Dmitrii Slavíček, Petr Spinlove, K. Eryn Vindel-Zandbergen, Patricia Agostini, Federica Bonella, Sara Martínez, Todd J. Worth, Graham A. Curchod, Basile F. E. |
| contents | This Perspective is part of a Special Topic that explored the maturity of nonadiabatic molecular dynamics for predicting photochemical processes. In 2023, a prediction challenge was issued to the community of computational photochemists to simulate the photochemistry of cyclobutanone, photoexcited at 200 nm, and the resulting time-resolved MeV-UED signal. The challenge attracted 15 theoretical predictions from more than 70 researchers, employing a wide range of strategies for electronic structure and nonadiabatic molecular dynamics to predict the time-resolved MeV-UED signal before the experiment had been conducted at SLAC (Stanford, USA). The MeV-UED instrument at Shanghai Jiao Tong University was also used to provide a second independent time-resolved MeV-UED signal for the photochemistry of cyclobutanone.
This Perspective discusses the various approaches and strategies used by the participants to predict the photochemistry of cyclobutanone. This work also summarizes the strengths and weaknesses of various methods used for photoexcitation, electronic structure, nonadiabatic dynamics, and calculation of observables, as agreed by the participants during a CECAM workshop dedicated to the results of the challenge and organized in Lausanne in April 2025. This Perspective also collects all the predicted time-resolved MeV-UED signals into a single figure, together with the experimental signal. This challenge (i) demonstrated the qualitative predictive power of nonadiabatic molecular dynamics and (ii) underscore the impact of electronic-structure theory on the outcome of the excited-state dynamics and the need for its careful benchmarking. This effort allowed the community to share practical strategies to perform nonadiabatic dynamics (discussed in the present Perspective) and constitutes a 'calibration' exercise for computational photochemistry. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2604_12749 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | Perspective on a challenge: predicting the photochemistry of cyclobutanone Janoš, Jiří List, Nanna Holmgaard Orr-Ewing, Andrew J. Suchan, Jiří Barbatti, Mario Bennett, Olivia Brady, Marcus Carmona-García, Javier Crespo-Otero, Rachel Eng, Julien Fajen, O. Jonathan Garavelli, Marco Gómez, Sandra Green, Alice E. Hernández, Federico J. Hollas, Daniel Hutton, Lewis Ibele, Lea M. Kirrander, Adam Lan, Zhenggang Lassmann, Yorick Lawrence, Joseph E. Levine, Benjamin G. Makhov, Dmitry V. Mannouch, Jonathan R. Miao, Xincheng Mitrić, Roland Parker, Shane M. Penfold, Thomas J. Peng, Jiawei Richardson, Jeremy O. Shalashilin, Dmitrii Slavíček, Petr Spinlove, K. Eryn Vindel-Zandbergen, Patricia Agostini, Federica Bonella, Sara Martínez, Todd J. Worth, Graham A. Curchod, Basile F. E. Chemical Physics This Perspective is part of a Special Topic that explored the maturity of nonadiabatic molecular dynamics for predicting photochemical processes. In 2023, a prediction challenge was issued to the community of computational photochemists to simulate the photochemistry of cyclobutanone, photoexcited at 200 nm, and the resulting time-resolved MeV-UED signal. The challenge attracted 15 theoretical predictions from more than 70 researchers, employing a wide range of strategies for electronic structure and nonadiabatic molecular dynamics to predict the time-resolved MeV-UED signal before the experiment had been conducted at SLAC (Stanford, USA). The MeV-UED instrument at Shanghai Jiao Tong University was also used to provide a second independent time-resolved MeV-UED signal for the photochemistry of cyclobutanone. This Perspective discusses the various approaches and strategies used by the participants to predict the photochemistry of cyclobutanone. This work also summarizes the strengths and weaknesses of various methods used for photoexcitation, electronic structure, nonadiabatic dynamics, and calculation of observables, as agreed by the participants during a CECAM workshop dedicated to the results of the challenge and organized in Lausanne in April 2025. This Perspective also collects all the predicted time-resolved MeV-UED signals into a single figure, together with the experimental signal. This challenge (i) demonstrated the qualitative predictive power of nonadiabatic molecular dynamics and (ii) underscore the impact of electronic-structure theory on the outcome of the excited-state dynamics and the need for its careful benchmarking. This effort allowed the community to share practical strategies to perform nonadiabatic dynamics (discussed in the present Perspective) and constitutes a 'calibration' exercise for computational photochemistry. |
| title | Perspective on a challenge: predicting the photochemistry of cyclobutanone |
| topic | Chemical Physics |
| url | https://arxiv.org/abs/2604.12749 |