The intramolecular dynamic behavior of the tetrahedrane-type cluster [Fe 2 (CO) 6 (µ-SNH)] 1 was studied by 13 C NMR spectroscopy. The 57 Fe chemical shift of 1 and the coupling constants 1 J( 57 Fe, 13 C) were measured. These NMR parameters, and also 1 J( 57 Fe, 15 N), were found to be in good agreement with data calculated by using density functional theory (DFT) methods (B3LYP), based on the geometry calculated at the 6-311 + G(d,p) level of theory. The isolobal replacement of the Fe(CO) 3 with BH fragments leads to the tetrahedranes [Fe(CO) 3 (BH)(µ-SNH)] 2 and [(HB) 2 (µ-SNH)] 3. Both were identified by calculations as minima on the respective potential energy surface (PES). However, the tetrahedrane-type structure of 3 is much higher in energy when compared with the planar cyclic isomers 3a and 3b.