Femtosecond spectroscopy and quantum chemical molecular dynamics simulations of photoinduced proton transfer processes in aqueous solution

水溶液中光致质子转移过程的飞秒光谱和量子化学分子动力学模拟

• 批准号: 263266015
• 负责人: Dr. Erik T.J. Nibbering
• 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
• 资助国家: 德国
• 项目状态: 未结题
• 来源: https://gepris.dfg.de/gepris/projekt/263266015?language=en
• 关键词: Femtosecond; spectroscopy; quantum; chemical; molecular

We explore the atomistic protonation pathways of acid-base proton exchange reactions in aqueous solution by means of a joint experimental and theoretical approach. Particular focus is put on the specific nature of the transfer reaction (cation versus anion versus combined anion/cation dynamics) and on the dependence on the chemistry of the involved co-solvent molecules (kosmotropic/chaotropic salts and molecules).The proton exchange reaction is triggered by optical activation of a photo-acid and spectroscopically analyzed via time-resolved femtosecond UV pump-probe spectroscopy. In parallel, quantum chemical molecular dynamics simulations are combined with IR fingerprint calculations of transient structural motifs from the proton exchange trajectories.

我们通过实验和理论相结合的方法探索了水溶液中酸碱质子交换反应的原子质子化途径。特别关注的是把转移反应的具体性质（阳离子与阴离子与阴离子/阳离子相结合的动力学）和对所涉及的共溶剂分子（kosmotropic/chaotropic盐和分子）的化学的依赖性。质子交换反应是由光酸的光活化和光谱分析通过时间分辨飞秒紫外泵浦-探测光谱。并行，量子化学分子动力学模拟相结合的瞬态结构图案的质子交换轨迹的红外指纹计算。