Wang Jun, Gao Shu Ning, Liu Aihua, He Lanhai, Zhao Xi
Institute of Atomic and Molecular Physics, Jilin University, Changchun, 130012, People's Republic of China.
School of Physics and Information Technology, Shaanxi Normal University, Xi'an, 710062, Shaanxi, People's Republic of China.
Sci Rep. 2025 Jan 2;15(1):117. doi: 10.1038/s41598-024-83209-6.
Electron-nuclear coupling plays a crucial role in strong laser induced molecular dissociation dynamics. The interplay between electronic and nuclear degrees of freedom determines the pathways and outcomes of molecular fragmentation. However, a full quantum mechanical treatment of electron-nuclear dynamics is computationally intensive. In this work, we have developed a Strong Laser Induced non-adiabatic Multi-Ionic-Multi-Electric States (SLIMIMES) approach, which contains the electron-laser and electron-nuclear couplings. We validate our model using a showcase example: water dissociation under strong infrared (IR) laser pulses. Our investigation reveals the predominant role of a non-vertical dissociation pathway in the photo-ionization dissociation (PID) process of [Formula: see text]. This pathway originates from neutral [Formula: see text], which undergoes vertical multi-photon-single-ionization, reaching the intermediate dissociation states of [Formula: see text] within [Formula: see text]. Subsequently, [Formula: see text] dissociates into [Formula: see text], with both [Formula: see text] and [Formula: see text] fragments potentially ionizing an electron during interaction with the IR laser. This sequential PID pathway significantly contributes to the dissociation yields of water dication. Our calculations are consistent with recent experimental data, which focus on measuring the branching ratio of water dication dissociation. We aim for our model to provide a deeper understanding and a fresh perspective on the coupling between electron and nuclear dynamics induced by a strong IR laser field.
电子 - 核耦合在强激光诱导的分子解离动力学中起着至关重要的作用。电子和核自由度之间的相互作用决定了分子碎片化的途径和结果。然而，对电子 - 核动力学进行完全量子力学处理在计算上是密集的。在这项工作中，我们开发了一种强激光诱导的非绝热多离子 - 多电态（SLIMIMES）方法，该方法包含电子 - 激光和电子 - 核耦合。我们使用一个展示示例来验证我们的模型：强红外（IR）激光脉冲下的水分解。我们的研究揭示了非垂直解离途径在[化学式：见原文]的光电离解离（PID）过程中的主导作用。这条途径起源于中性的[化学式：见原文]，它经历垂直多光子单电离，在[时间范围：见原文]内达到[化学式：见原文]的中间解离态。随后，[化学式：见原文]分解为[化学式：见原文]，在与红外激光相互作用期间，[化学式：见原文]和[化学式：见原文]碎片都可能使一个电子电离。这种顺序PID途径对水二价阳离子的解离产率有显著贡献。我们的计算与最近专注于测量水二价阳离子解离分支比的实验数据一致。我们的目标是让我们的模型为强红外激光场诱导的电子与核动力学之间的耦合提供更深入的理解和全新的视角。
