Auger electron spectroscopy as a probe of ion pairing and protonation effects in aqueous solutions

俄歇电子能谱作为水溶液中离子配对和质子化效应的探针

• 批准号: 107745161
• 负责人: Professor Dr. Lorenz S. Cederbaum
• 金额: --
• 依托单位: Forschungsgruppe Theoretische Chemie
• 依托单位国家: 德国
• 项目类别: Research Grants
• 财政年份: 2009
• 资助国家: 德国
• 起止时间: 2008-12-31 至 2016-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/107745161?language=en
• 关键词: Auger; electron; spectroscopy; probe; ion

Auger electron spectroscopy (AES) is a powerful technique for investigating matter, recently came into use also for studying liquids. Being an extremely sensitive and informative tool to probe electronic and geometric structures of systems under study, AES has a great potential for elucidating solvation phenomena whose microscopic details are still rather poorly understood. Comprehensive theoretical studies of Auger spectra of aqueous solutions are unavailable nowadays and our project is intended to make up for this deficiency. We plan to calculate Auger spectra of different clusters of hydrated salts, bases and acids to gain deep insight into the interactions operative in bulk solutions at the microscopic level. The evolution of spectra with cluster size and the dependence on various choices of counter ions will be carefully examined and explained. Our preliminary calculations have already revealed that many peculiarities of the experimental Auger spectra of bulk aqueous solutions have their analogs in the spectra of microsolvated clusters. The clusters are accessible to ab initio studies and can be considered as invaluable model systems of bulk aqueous solutions. Based on the ab initio calculations we ultimately hope to derive a semi-empirical model for describing various solvent effects in the Auger spectra of ionic compounds.

俄歇电子能谱(AES)是研究物质的一种强有力的技术，最近也被用于研究液体。俄歇电子能谱是一种极其灵敏和信息丰富的工具，用于探测所研究体系的电子结构和几何结构，在解释溶剂化现象方面有很大的潜力，而溶剂化现象的微观细节仍然知之甚少。目前还没有对水溶液的俄歇光谱进行全面的理论研究，我们的项目就是为了弥补这一不足。我们计划计算不同水合盐、碱和酸簇的俄歇光谱，以在微观水平上深入了解主体溶液中的相互作用。我们将仔细研究和解释光谱随团簇大小的演变以及对不同反离子选择的依赖。我们的初步计算表明，体水溶液的实验俄歇光谱的许多特性与微溶剂化团簇的光谱有相似之处。这些团簇可用于从头算研究，并且可以被认为是无价的大块水溶液的模型系统。在从头计算的基础上，我们最终希望得到一个描述离子化合物俄歇光谱中各种溶剂效应的半经验模型。

项目成果

Microhydration of LiOH: Insight from electronic decays of core-ionized states.

LiOH 的微水合：核心电离态电子衰变的见解

• DOI: 10.1063/1.4954661
• 发表时间: 2016
• 期刊: The Journal of chemical physics
• 作者: Kryzhevoi N.V.

Relaxation Processes in Aqueous Systems upon X-ray Ionization: Entanglement of Electronic and Nuclear Dynamics.

• DOI: 10.1021/acs.jpclett.5b02665
• 发表时间: 2016-01
• 期刊: The journal of physical chemistry letters
• 作者: P. Slavíček;N. Kryzhevoi;E. F. Aziz;B. Winter

Observation of electron-transfer-mediated decay in aqueous solution.

水溶液中电子转移介导的衰变的观察

• DOI: 10.1038/nchem.2727
• 发表时间: 2017
• 期刊: Nature chemistry
• 影响因子: 21.8
• 作者: Unger I;Seidel R;Thürmer S;Pohl M.N;Aziz E.F;Cederbaum L.S;Muchová E;Slavíček P;Winter B;Kryzhevoi N.V.
• 通讯作者: Kryzhevoi N.V.

Proton-transfer mediated enhancement of nonlocal electronic relaxation processes in X-ray irradiated liquid water.

质子转移介导的 X 射线照射液态水中非局域电子弛豫过程的增强

• DOI: 10.1021/ja5117588
• 发表时间: 2014
• 期刊: Journal of the American Chemical Society
• 影响因子: 15
• 作者: Slavíček P;Winter B;Cederbaum L.S;Kryzhevoi N.V.
• 通讯作者: Kryzhevoi N.V.

Ultrafast Charge Transfer Processes Accompanying KLL Auger Decay in Aqueous KCl Solution.

KCl 水溶液中伴随 KLL 俄歇衰变的超快电荷转移过程

• DOI: 10.1103/physrevlett.119.263003
• 发表时间: 2017
• 期刊: Physical review letters
• 影响因子: 8.6
• 作者: Céolin D;Kryzhevoi N.V;Nicolas Ch;Pokapanich W;Choksakulporn S;Songsiriritthigul P. Saisopa T;Rattanachai Y;Utsumi Y;Palaudoux J;Öhrwall G;Rueff J.P.
• 通讯作者: Rueff J.P.