Electronic structure and dynamics of solvated chromophores: femtosecond photoelectron spectroscopy from a liquid water jet

溶剂化发色团的电子结构和动力学：来自液态水射流的飞秒光电子能谱

• 批准号: 167377349
• 负责人: Dr. Andrea Lübcke
• 金额: --
• 依托单位: Max-Born-Institut für Nichtlineare Optik und Kurzzeitspektroskopie (MBI)
• 依托单位国家: 德国
• 项目类别: Research Grants
• 财政年份: 2011
• 资助国家: 德国
• 起止时间: 2010-12-31 至 2015-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/167377349?language=en
• 关键词: Electronic; structure; dynamics; solvated; chromophores

Time-resolved photoelectron spectroscopy (TRPES) allows the direct observation of transient electronic structure in atoms and molecules, and was very successful in probing structure and dynamics of gas-phase molecules and surfaces. Based on the recent development of liquid-jet photoelectron spectroscopy in our institute, we propose now to study time-resolved photoelectron spectra of solvated molecules in a liquid jet. Photophysical and photochemical processes in solvated chomophores will be initiated by ultraviolet or visible fs laser pulses and probed by time-delayed photoionization of valence electrons, projecting the electronic structure into the ionization continuum. A liquid-jet source was designed following proven designs and is combined with a magnetic bottle spectrometer suited for the detection of electrons with low kinetic energies (0-10 eV). Experiments will characterize charge-transfer-to-solvent (CTTS) and internal conversion processes in model chromophores. We will attempt to identify dominant solute-solvent interactions by comparison to gas-phase and cluster data and corresponding ab initio theory.

时间分辨的光电子光谱（TRPE）可以直接观察原子和分子中的瞬态电子结构，并且在探测结构和气相分子和表面的动力学方面非常成功。基于我们研究所液体射流光谱光谱的最新发展，我们现在建议研究液体射流中溶剂化分子的时间分辨光电光谱。溶剂化的CHOMOPHORES中的光物理和光化学过程将由紫外线或可见的FS激光脉冲启动，并通过对价电子的时间删除光电离心进行探测，将电子结构投射到电离连续体中。在经过验证的设计之后设计了液体喷射源，并与适合检测低动能能量（0-10 eV）的电子的磁性瓶光谱仪结合使用。实验将表征模型发色团中的电荷转移到溶剂（CTT）和内部转换过程。我们将尝试通过与气相和群集数据以及相应的从头算理论进行比较来确定主要的溶质 - 溶剂相互作用。

项目成果

Role of alkali cations for the excited state dynamics of liquid water near the surface.

碱金属阳离子对表面附近液态水激发态动力学的作用

• DOI: 10.1063/1.4732582
• 发表时间: 2012
• 期刊: The Journal of chemical physics
• 作者: F. Buchner;H. H. Ritze;M. Beutler;T. Schultz;I. V. Hertel;A. Lübcke
• 通讯作者: A. Lübcke