Photoionisation-induced switch in aromatic molecule-solvent recognition

芳香族分子溶剂识别中的光电离诱导开关

• 批准号: 165827969
• 负责人: Professor Dr. Otto Dopfer
• 金额: --
• 依托单位: Arbeitsgruppe Lasermolekülspektroskopie und Umweltphysik (AG Dopfer)
• 依托单位国家: 德国
• 项目类别: Research Grants
• 财政年份: 2010
• 资助国家: 德国
• 起止时间: 2009-12-31 至 2017-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/165827969?language=en
• 关键词: Photoionisation; induced; switch; aromatic; molecule

This project aims at the infrared (IR) spectroscopic and quantum chemical characterization of aromatic ion-ligand complexes isolated in the gas phase, in order to determine the potential energy surface describing the involved intermolecular ion-ligand interaction in the electronic ground state. Target molecules are cations of fundamental benzene derivatives of biophysical relevance, which are microsolvated by a controlled number of neutral solvent molecules. In a collaborative effort, two unique but complementary experimental strategies are combined to characterize the intermolecular potential by generating the clusters with two different techniques in a molecular beam. The first approach employs electron impact ionisation for cluster generation, which enables the characterization of the global minima on the potential. In a second approach, the cation clusters are generated by resonant photoionisation (REMPI) of the neutral precursor. As the interaction potential of the neutral and ionic clusters are qualitatively different (due to the additional charge), higher-lying local minima on the potential of the cation ground state can be populated by REMPI and characterized by IR spectroscopy. Depending on the excess energy involved in the ionisation process and the magnitude of the barrier for isomerisation, the local minima will isomerise toward the global minima. The dynamics of this ionisation-induced isomerisation process will directly be measured by time-resolved IR spectroscopy. The shape of the intermolecular potential and the dynamics of this reorganization process will be investigated as a function of the substitution of functional groups, the excess energy involved in ionisation, and the type and degree of microsolvation.

该项目旨在对气相中分离的芳香族离子-配体复合物进行红外光谱和量子化学表征，以确定描述电子基态中所涉及的分子间离子-配体相互作用的势能面。靶分子是生物物理相关的基本苯衍生物的阳离子，其被受控数量的中性溶剂分子微溶剂化。在一个合作的努力，两个独特的，但互补的实验策略相结合，以表征分子间的潜力，通过产生集群与两种不同的技术在分子束。第一种方法采用电子碰撞电离集群生成，这使得表征的全球最小的潜力。在第二种方法中，通过中性前体的共振光电离（REMPI）产生阳离子簇。由于中性和离子簇的相互作用势是定性不同的（由于额外的电荷），较高的躺在本地的最小值的阳离子基态的电位可以填充由REMPI和其特征在于由IR光谱。取决于电离过程中涉及的过剩能量和异构化势垒的大小，局部极小值将向全局极小值异构化。这种电离诱导的异构化过程的动力学将直接通过时间分辨红外光谱测量。的形状的分子间的潜力和这个重组过程的动力学将被调查作为功能的功能基团的取代，参与电离的过剩能量，和微溶剂化的类型和程度。

项目成果

Watching water migration around a peptide bond.

• DOI: 10.1002/anie.201203296
• 发表时间: 2012-07
• 期刊: Angewandte Chemie
• 作者: Kohei Tanabe;M. Miyazaki;M. Schmies;A. Patzer;Markus Schütz;H. Sekiya;M. Sakai;O. Dopfer;M. Fujii

Ionisation-induced site switching dynamics in solvated aromatic clusters: phenol–(rare gas) n clusters as prototypical example

溶剂化芳香族簇中电离诱导的位点切换动力学：苯酚（稀有气体）n簇作为典型例子

• DOI: 10.1080/0144235x.2012.656013
• 发表时间: 2012
• 期刊: International Reviews in Physical Chemistry
• 影响因子: 6.1
• 作者: M. Fujii;O. Dopfer
• 通讯作者: O. Dopfer

Mass analyzed threshold ionization detected infrared spectroscopy: isomerization activity of the phenol-Ar cluster near the ionization threshold.

质量分析阈值电离检测红外光谱：苯酚-Ar簇在电离阈值附近的异构化活性

• DOI: 10.1039/c4cp04584j
• 发表时间: 2015
• 期刊: Physical chemistry chemical physics : PCCP
• 作者: M. Miyazaki;S. Yoshikawa;F. Michels;K. Misawa;S. Ishiuchi;M. Sakai;O. Dopfer;K. Müller-Dethlefs;M. Fujii
• 通讯作者: M. Fujii

Deciphering environment effects in peptide bond solvation dynamics by experiment and theory.

通过实验和理论解读肽键溶剂化动力学中的环境影响

• DOI: 10.1039/c7cp03992a
• 发表时间: 2017
• 期刊: Physical chemistry chemical physics : PCCP
• 作者: M. Wohlgenuth;M. Miyazaki;K. Tsukuda;M. Weiler;O. Dopfer;M. Fujii;R. Mitric
• 通讯作者: R. Mitric

Microhydrated aromatic cluster cations: binding motifs of 4-aminobenzonitrile-(H₂O)n cluster cations with n ≤ 4.

微水合芳香族簇阳离子：4-氨基苯甲腈-(HâO)n簇阳离子的结合基序，n≤4

• DOI: 10.1063/1.4901893
• 发表时间: 2014
• 期刊: The Journal of chemical physics
• 作者: M. Schmies;M. Miyazaki;M. Fujii;O. Dopfer
• 通讯作者: O. Dopfer