Dissociation and ionization of diatomic molecules in laser fields - full dimensional ab-initio description including electron-nuclear correlations

激光场中双原子分子的解离和电离 - 全维从头计算描述，包括电子-核相关性

• 批准号: 280059503
• 负责人: Professor Dr. Rüdiger Schmidt (†)
• 金额: --
• 依托单位: Max-Planck-Institut für Kernphysik
• 依托单位国家: 德国
• 项目类别: Research Grants
• 财政年份: 2015
• 资助国家: 德国
• 起止时间: 2014-12-31 至 2019-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/280059503?language=en
• 关键词: Dissociation; ionization; diatomic; molecules; laser

The concern of this project is the extension of the recently developed "Non-Adiabatic Quantum Molecular Dynamics with Hopping" (NA-QMD-H) method to explicitly include an external laser field in the theoretical description during the molecular dynamics in harmonic, arbitrary long pulses. The new approach allows for an full-dimensional (including rotation, vibration, and electronic excitation) simultaneous ab-initio description of the laser-driven dissociation and ionization of two-atomic molecules, including quantum effects in the nuclear dynamics. This approach therefore is an approximative solution of the full time-dependend Schrödinger equation for electrons and nuclei. It is the ultimate goal of many years of development of Dresden's NA-QMD method (see Section "Eigene Vorarbeiten"). This goal shall be achieved with an approximate quantum-mechanical treatment of the nuclei, where classical trajectories are propagated on quantum-mechanically determined energy surfaces. The choice of these surfaces is crucical. In the intended method, Floquet surfaces (during the pulse) and Born-Oppenheimer surfaces (for the relaxation dynamics following the pulse) will be applied. In connection with quantum-mechanically determined transition rates between single surfaces ("hopping"), this should allow for an accurate description of the laser-driven molecular dynamics including electron-nuclear correlations. For H2+, we already have experience with this approach. The challenging extension of the method to two-atomic multi-electron molecules is the narrower concern of the present project. For the first time, density-functional-theory-Floquet surfaces of the Kohn-Sham system corresponding to the molecule shall be used here. A further new and important point of the method is the description of photoionization by hopping between surfaces of the neutral, single, or multiple ionized molecule, such that a complete description of all (relevant) ionization channels should be possible.For this project a cooperation agreement with the Max-Planck-Institut für Kernphysik (MPIK) Heidelberg has been concluded (see attachments). At the MPIK, kinematically complete experiments concerning the dissociation and ionization are performed using a reaction microscope. In consultation with the MPIK, specific calculations shall be done at first for argon dimers (later also for other noble gases as well as O2 and N2), the results shall be compared to the experimental findings and help with their interpretation. Furthermore, simulations for the interpretation of pump-probe experiments are planned. The new method allows for an explicit inclusion of the pump and the probe pulse in the calculation. A common aim, among others, is to investigate to what extent the molecular dynamics can be manipulated by suitable choices of the laser parameters.

关注最近开发的“使用Hoth Hoth Hothod）方法的“非生成分子动力学”方法明确包含了谐波，任意长脉冲的分子动力学期间理论上的外部激光场。新方法全约合（新方法）激光驱动的解散和两种原子分子的电离的旋转，振动和电子迁移）在核动力学中不量量子效应。 F Dressden的NA-QMD方法的开发（请参阅“ Egene vorarbeiten”部分。在预期的方法中，表面是弯曲的。 ），这应该允许对激光驱动的分子动力学进行准确的描述，包括电子核的相关性首次使用中性，单个或多个电离分子的kohn-sham系统的密度功能性浮力表面。对于这个项目，与Max-Planck-institutfürKernphysik（MPIK）Heidelberg达成了合作协议（请参阅MPIK的附件）与MPIK进行咨询，应将特定的计算与Argon Dimers Ts进行，并在这里进行解释。可以通过适当的激光参数选择来调查分子动力学。