Silver‐Templated γ‐Keggin Alkyltin‐Oxo Cluster: Electronic Structure and Optical Limiting Effect

As one of the most representative polyoxometalate (POM) structures, Keggin clusters have attracted considerable attention. Nevertheless, the noble‐metal‐templated Keggin structure has not been reported to date. In this work, for the first time, a Ag atom was successfully incorporated to template the...

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Published inAngewandte Chemie International Edition Vol. 61; no. 27; pp. e202202853 - n/a
Main Authors Zhu, Yu, Wang, Zirui, Li, Dejing, Zhu, Yin‐Di, Li, Qiao‐Hong, Li, Dong‐Sheng, Zhang, Lei
Format Journal Article
LanguageEnglish
Published Germany Wiley Subscription Services, Inc 04.07.2022
EditionInternational ed. in English
Subjects
Clusters
Constraining
Electron transfer
Electronic Structure
Keggin Structures
Molecular orbitals
Noble metals
Nonlinear optics
Optical Limiting
Optical properties
Polyoxometallates
Silver
Tin-Oxo Clusters
Electronic Structure
Silver
Tin-Oxo Clusters
Keggin Structures
Optical Limiting
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Summary:As one of the most representative polyoxometalate (POM) structures, Keggin clusters have attracted considerable attention. Nevertheless, the noble‐metal‐templated Keggin structure has not been reported to date. In this work, for the first time, a Ag atom was successfully incorporated to template the formation of a γ‐Keggin alkytin‐oxo cluster. Moreover, the central Ag atom has brought a significant heavy atom effect, showing the important influence on the electronic structure and optical properties. Theoretical calculations demonstrate that the Ag atom affects the frontier molecular orbitals and excited states of the AgSn12 cluster, and also the process of electron transfer. The solid structure of the AgSn12 cluster exhibits a significant third‐order nonlinear optical (NLO) response, and an excellent optical limiting effect has been experimentally verified. The success of this work opens the way for the construction and optical properties modulation of noble metal templated Keggin structures. The first noble‐metal‐templated Keggin structure, AgSn12, is prepared. The central Ag atom significantly influences the electronic structure and optical properties of the whole cluster, which have been investigated by theoretical calculations and Z‐scan measurements.
Bibliography:These authors contributed equally to this work.
co‐first authors
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ISSN:1433-7851
1521-3773
1521-3773
DOI:10.1002/anie.202202853