The Ga(84)R(20)(4-) [R = N(SiMe(3))(2)] species, which represents the largest metalloid cluster entity structurally characterized so far, has been electronically and topologically modified: Via changing the redox potential of the reaction solution, crystals different from those containing the Ga(84)R(20)(4-) anion can be isolated, featuring similar Ga(84)R(20)(3-) entities. An accurate crystal structure analysis via synchrotron radiation is presented, which might be the first step toward an understanding of the metallic conductivity and superconductivity of the Ga(84)R(20)(4-) cluster compound, physical properties which are singular in the field of metalloid clusters so far.

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