Charge-directed reactivity of molecules and its control by short laser pulses

分子的电荷定向反应及其短激光脉冲的控制

• 批准号: 281241953
• 负责人: Professor Dr. Alexander Kuleff
• 金额: --
• 依托单位: Forschungsgruppe Theoretische Chemie
• 依托单位国家: 德国
• 项目类别: Priority Programmes
• 财政年份: 2015
• 资助国家: 德国
• 起止时间: 2014-12-31 至 2021-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/281241953?language=en
• 关键词: Charge; directed; reactivity; molecules; its

Exposing molecules to ultrashort laser pulses can trigger pure electron dynamics in the excited or ionized system. In the case of ionization, these dynamics may manifest as an ultrafast migration of the initially created hole-charge throughout the system and were termed charge migration. Due to the coupling between the electronic and the nuclear motion, the control over the pure electron dynamics offers the extremely interesting possibility to steer the succeeding chemical reactivity by predetermining the reaction outcome at a very early stage.That is why, the charge-migration phenomenon increasingly attracts the attention of the scientific community and at present several groups are preparing experiments to study the process using novel attosecond pulse techniques. In the first period of this project we developed schemes and protocols that allow to design ultrashort laser pulses that can efficiently control the electronic charge migration process in polyatomic molecules.The main goal of the renewal project is to develop methodologies allowing to treat purely quantum mechanically the coupled electron-nuclear dynamics of moderate size molecular cations in the presence of a laser field and to apply this methodology to experimentally interesting systems.This will allow to answer the key question of attochemistry, namely can we steer chemical reactions in molecular cations by manipulating the pure electronic charge-migration step. Such calculations will, on onehand, provide the experimentalists the needed conceptual understanding and help in interpreting the experimental results, and,on the other hand, will guide future experimental efforts by proposing interesting systems and effects to be measured.

将分子暴露于超短激光脉冲可以在激发或电离系统中触发纯电子动力学。在电离的情况下，这些动力学可以表现为最初产生的空穴电荷在整个系统中的超快迁移，并被称为电荷迁移。由于电子和核运动之间的耦合，对纯电子动力学的控制提供了非常有趣的可能性，通过在非常早期的阶段预先确定反应结果来引导随后的化学反应。控罪─迁移现象越来越引起科学界的注意，目前有几个小组正在准备实验，利用新的阿秒来研究这一过程脉冲技术在该项目的第一阶段，我们开发了允许设计超短激光脉冲的方案和协议，这些激光脉冲可以有效地控制多原子分子中的电子电荷迁移过程。更新项目的主要目标是开发允许纯量子力学处理耦合电子的方法。在激光场的存在下，中等大小的分子阳离子的核动力学，并将这种方法应用于实验感兴趣的系统。这将允许回答的关键问题，原子化学，即我们可以通过操纵纯电子电荷迁移步骤来操纵分子阳离子中的化学反应。这样的计算一方面将为实验者提供必要的概念性理解，并有助于解释实验结果，另一方面，将通过提出需要测量的有趣系统和效应来指导未来的实验工作。