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Here, we report a tetrahedral silver(I) cluster of Ag44+ covered by Δ-[Rh(l-cys)3]3- (l-H2cys = l-cysteine), which is converted to an Ag4H3+ cluster via the inclusion of a H- ion. The 11 reaction of Δ-[Rh(l-cys)3]3- with Ag+ gave a sulfur-bridged AgI4RhIII4 octanuclear structure in [Ag4Rh(l-cys)34]8- ([1]8-), in which a tetrahedral Ag44+ core is bound by four Δ-[Rh(l-cys)3]3- units through thiolato groups. DFT calculations revealed that a superatomic orbital exists in Ag44+ as the lowest unoccupied molecular orbital, contributing to the app
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