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在水性环境中对核心离子化物种进行有效中和。

Efficient neutralization of core ionized species in an aqueous environment.

作者信息

Pelimanni Eetu, Hans Andreas, Heikura Emilia, Huttula Marko, Patanen Minna

机构信息

Nano and Molecular Systems Research Unit, Faculty of Science, University of Oulu, Box 3000, FI-90014, Finland.

Universität Kassel, Institut für Physik und CINSaT, Heinrich-Plett-Straße 40, 34132, Kassel, Germany.

出版信息

Phys Chem Chem Phys. 2022 May 18;24(19):11646-11653. doi: 10.1039/d2cp01178f.

Abstract

Core ionization dynamics of argon-water heteroclusters Ar[HO] are investigated using a site and process selective experimental scheme combining 3 keV electron irradiation with Auger electron-ion-ion multi-coincidence detection. The formation of Ar 2p vacancies followed by non-radiative decay to intermediate one-site doubly ionized states Ar(3p)-Ar[HO] and subsequent redistribution of charge to the cluster environment are monitored. At low argon concentrations the emission of an [HO]H/[HO]H ion pair is the dominant outcome, implying on high efficiency of charge transfer to the water network. Increasing the condensation fraction of argon in the mixed clusters and/or to pure argon clusters is reflected as a growing yield of Ar/Ar ion pairs, providing a fingerprint of the precursor heterocluster beam composition. The coincident Auger electron spectra, resolved with better than 1 eV resolution, show only subtle differences and thereby reflect the local nature of the initial Auger decay step. The results lead to better understanding of inner shell ionization processes in heterogeneous clusters and in aqueous environments in general.

摘要

利用一种将3 keV电子辐照与俄歇电子-离子-离子多重符合探测相结合的位点和过程选择性实验方案,研究了氩-水异质团簇Ar[HO]的核心电离动力学。监测了Ar 2p空位的形成,随后通过无辐射衰变到中间的单位点双电离态Ar(3p)-Ar[HO],以及随后电荷向团簇环境的重新分布。在低氩浓度下,[HO]H/[HO]H离子对的发射是主要结果,这意味着电荷转移到水网络的效率很高。混合团簇中氩的冷凝分数增加和/或变为纯氩团簇,表现为Ar/Ar离子对产率的增加,这提供了前体异质团簇束组成的一个特征。具有优于1 eV分辨率的符合俄歇电子能谱仅显示出细微差异,从而反映了初始俄歇衰变步骤的局部性质。这些结果有助于更好地理解一般情况下异质团簇和水环境中的内壳层电离过程。

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