Cigrang Léon L E, Curchod Basile F E, Ingle Rebecca A, Kelly Aaron, Mannouch Jonathan R, Accomasso Davide, Alijah Alexander, Barbatti Mario, Chebbi Wiem, Došlić Nadja, Eklund Elliot C, Fernandez-Alberti Sebastian, Freibert Antonia, González Leticia, Granucci Giovanni, Hernández Federico J, Hernández-Rodríguez Javier, Jain Amber, Janoš Jiří, Kassal Ivan, Kirrander Adam, Lan Zhenggang, Larsson Henrik R, Lauvergnat David, Le Dé Brieuc, Lee Yeha, Maitra Neepa T, Min Seung Kyu, Peláez Daniel, Picconi David, Qiu Zixing, Raucci Umberto, Robertson Patrick, Sangiogo Gil Eduarda, Sapunar Marin, Schürger Peter, Sinnott Patrick, Tretiak Sergei, Tikku Arkin, Vindel-Zandbergen Patricia, Worth Graham A, Agostini Federica, Gómez Sandra, Ibele Lea M, Prlj Antonio
Department of Chemistry, University College London, 20 Gordon St., WC1H 0AJ London, United Kingdom.
Centre for Computational Chemistry, School of Chemistry, University of Bristol, Bristol BS8 1TS, United Kingdom.
J Phys Chem A. 2025 Aug 7;129(31):7023-7050. doi: 10.1021/acs.jpca.5c02171. Epub 2025 Jul 15.
Simulating the coupled electronic and nuclear response of a molecule to light excitation requires the application of nonadiabatic molecular dynamics. However, when faced with a specific photophysical or photochemical problem, selecting the most suitable theoretical approach from the wide array of available techniques is not a trivial task. The challenge is further complicated by the lack of systematic method comparisons and rigorous testing on realistic molecular systems. This absence of comprehensive molecular benchmarks remains a major obstacle to advances within the field of nonadiabatic molecular dynamics. A CECAM workshop, , was held in May 2024 to address this issue. This Perspective highlights the key challenges identified during the workshop in defining molecular benchmarks for nonadiabatic dynamics. Specifically, this work outlines some preliminary observations on essential components needed for simulations and proposes a roadmap aiming to establish, as an ultimate goal, a community-driven, standardized molecular benchmark set.
模拟分子对光激发的电子和核耦合响应需要应用非绝热分子动力学。然而，面对特定的光物理或光化学问题时，从众多可用技术中选择最合适的理论方法并非易事。由于缺乏系统的方法比较以及对实际分子系统的严格测试，这一挑战变得更加复杂。缺乏全面的分子基准仍然是非绝热分子动力学领域进展的主要障碍。2024年5月举办了一次CECAM研讨会来解决这个问题。本观点文章强调了研讨会期间确定的在定义非绝热动力学分子基准方面的关键挑战。具体而言，这项工作概述了对模拟所需基本组件的一些初步观察，并提出了一个路线图，旨在最终建立一个由社区驱动的标准化分子基准集。
