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Lookup NU author(s): Dr Julien EngORCiD, Professor Thomas PenfoldORCiD
This work is licensed under a Creative Commons Attribution 4.0 International License (CC BY 4.0).
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 mega-electronvolt ultrafast electron diffraction (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. The challenge (i) demonstrated the qualitative predictive power of nonadiabatic molecular dynamics and (ii) underscored 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.
Author(s): Janos J, List NH, Orr-Ewing AJ, Suchan J, Barbatti M, Bennett O, Brady M, Carmona-Garcia J, Crespo-Otero R, Eng J, Fajen OJ, Garavelli M, Gomez S, Green AE, Hernández FJ, Hollas D, Hutton L, Ibele LM, Kirrander A, Lan Z, Lassmann Y, Lawrence JE, Levine BG, Makhov DV, Mannouch JR, Miao X, Mitric R, Parker SM, Penfold TJ, Peng J, Richardson JO, Shalashilin D, Slavicek P, Spinlove KE, Vindel-Zandbergen P, Agostini F, Bonella S, Martínez TJ, Worth GA, Curchod BFE
Publication type: Article
Publication status: Published
Journal: Journal of Chemical Physics
Year: 2026
Volume: 165
Issue: 2
Online publication date: 14/07/2026
Acceptance date: 11/06/2026
Date deposited: 21/07/2026
ISSN (print): 0021-9606
ISSN (electronic): 1089-7690
Publisher: API Publishing
URL: https://doi.org/10.1063/5.0338792
DOI: 10.1063/5.0338792
Data Access Statement: The data that support the findings of this study are openly available in Zenodo at https://doi.org/10.5281/zenodo.20559411.
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