反应性通量匹配:罕见事件的机制发现与自适应采样 / Reactive Flux Matching: Mechanism Discovery and Adaptive Sampling of Rare Events
1️⃣ 一句话总结
本文提出了一种名为“通量匹配”的新方法,它能够从分子模拟数据中自动提取出反应的关键路径和反应坐标,无需依赖任何预先设定的动力学模型,从而帮助科学家更高效地发现化学反应机制并提升对罕见事件的采样效率。
Path sampling methods generate ensembles of reactive trajectories connecting metastable states, but extracting mechanistic insight from these data remains nontrivial. We introduce Flux Matching, a framework that learns two complementary objects directly from reactive trajectory data: a current velocity $u(z)$, whose streamlines trace the dominant reaction pathways, and a scalar potential $h(z)$, obtained from a weighted Helmholtz-Hodge decomposition of the reactive current, that serves as a data-driven reaction coordinate. Both minimize quadratic functionals over the reactive path ensemble, analogous to the flow matching loss in generative modeling, and require no knowledge of the underlying dynamics or stationary distribution. Unlike committor-based methods, $u$ and $h$ remain well-defined under projection onto non-Markovian collective variables, and their level sets in turn provide adaptive interfaces for improved sampling with enhanced sampling methods. Flux Matching is validated through the generation of current velocity trajectories and rate constant calculations on molecular systems.
反应性通量匹配:罕见事件的机制发现与自适应采样 / Reactive Flux Matching: Mechanism Discovery and Adaptive Sampling of Rare Events
本文提出了一种名为“通量匹配”的新方法,它能够从分子模拟数据中自动提取出反应的关键路径和反应坐标,无需依赖任何预先设定的动力学模型,从而帮助科学家更高效地发现化学反应机制并提升对罕见事件的采样效率。
源自 arXiv: 2606.06295