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The reaction of dialkylzinc compounds R 2 Zn (R = Me, Et) with N,N-dimethylhydrazine and trimethylsilanol in a 4 : 2 : 2 ratio leads to the formation of tetra(alkylzinc) tris-siloxide monohydrazide aggregates, [(RZn) 4 (NHNMe 2 )(OSiMe 3 ) 3 ] [R = Me (1) and Et (2)]. These compounds are aggregates of mirror symmetry, containing the novel Zn 4 N 2 O 3  core. Both compounds have been characterised by  1 H,  13 C and  29 Si NMR and IR spectroscopy, by mass spectrometry and by elemental analysis, and 2 also by X-ray crystallography. The structure can be derived from a heterocubane, in which one anionic vertex is replaced by an NHNMe 2  group contributing two N atoms to the core constitution. By applying a ratio of hydrazine : silanol of 2 : 1 in a reaction with R 2 Zn (R = Me, Et, iPr), compounds of the general formula [(RZn) 4 (NHNMe 2 ) 2 (OSiMe 3 ) 2 ] [R = Me (3), Et (4), iPr (5)] are obtained. These aggregates contain a Zn 4 N 4 O 2  core. Upon employing a hydrazine : silanol ratio of 5 : 1 in a reaction with diisopropyl zinc, the compound [(iPrZn) 4 (NHNMe 2 ) 3 (OSiMe 3 )] results, containing a Zn 4 N 6 O unit. Compounds 3 - 6 have been characterised by  1 H,  13 C and  29 Si NMR and IR spectroscopy, by mass spectrometry and by elemental analysis. The topologic relationship between the pure hydrazides [(RZn) 4 (NHNMe 2 ) 4 ], the mixed aggregates [(RZn) 4 (NHNMe 2 ) 3 (OR’)], [(RZn) 4 (NHNMe 2 ) 2 (OR’) 2 ] and [(RZn) 4 (NHNMe 2 ) 3 (OR’) 3 ] and the pure alkoxides [(RZn) 4 (OR’) 4 ] is discussed.

Organozinc Siloxide-Hydrazide Aggregates [(RZn) 4 (NHNMe 2 ) x (OSiMe 3 ) (4 – x) ]