Abstract: The structures, physical properties, and reaction chemistry of isoelectronic alkyl complexes of osmium (V1) are compared. The three, five-coordinate alkyl complexes [NBun4][Os (N)(CH2SiMe3),], Os (NMe)(CH2SiMe3),, and Os (O)(CH, SiMe,), have been characterized by single-crystal X-ray diffraction, NMR, IR, UV-visible spectroscopy, and by electrochemical techniques. All have a square-pyramidal structure in the solid state, with ...