Guiot du Doignon Clément, Sinha-Roy Rajarshi, Rabilloud Franck, Despré Victor
Université Claude Bernard Lyon 1, CNRS, Institut Lumière Matière, UMR5306 F-69100 Villeurbanne France
Chem Sci. 2025 Aug 12. doi: 10.1039/d5sc02374b.
The possibility of observing correlation-driven charge migration has been a driving force behind theoretical and experimental developments in the field of attosecond molecular science since its inception. Despite significant accomplishments, the unambiguous experimental observation of this quantum beating remains elusive. In this work, we present a method to selectively trigger such dynamics in molecules predicted to exhibit long-lived electron coherence. We show that these dynamics can be selectively triggered using infrared multi-photon ionization and probed using the spacial resolution of X-ray free-electron laser, proposing a promising experimental scheme to study these pivotal dynamics. Additionally, we demonstrate that real-time time-dependent density-functional theory can describe correlation-driven charge migration resulting from a hole mixing structure involving the highest occupied molecular orbital of a molecule.
自阿秒分子科学领域创立以来，观测关联驱动的电荷迁移的可能性一直是该领域理论和实验发展的驱动力。尽管取得了重大成就，但这种量子拍频的明确实验观测仍然难以实现。在这项工作中，我们提出了一种方法，用于在预测会表现出长寿命电子相干性的分子中选择性地触发这种动力学。我们表明，可以使用红外多光子电离选择性地触发这些动力学，并利用X射线自由电子激光的空间分辨率进行探测，从而提出了一个研究这些关键动力学的有前景的实验方案。此外，我们证明了实时含时密度泛函理论可以描述由涉及分子最高占据分子轨道的空穴混合结构引起的关联驱动的电荷迁移。
