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The electronic absorption spectrum of the solid tetramethyl-ammonium salt of [OsO 2 (CN) 4 ] 2 -  is measured at 10 K. The five distinct band systems exhibit vibrational progressions in the range 660-750 cm  - 1 , corresponding to the Os = O stretching vibrations sometimes coupled with ν(OsC). From this vibrational fine structure the electronic origin is deduced and verified by characteristic isotopic shifts by  18 O and  13 C. The two bands at lowest energy are assigned to the d-d-transitions  1 A 1g  [b 2  2g ] →  3 E g  [b 1  2g  e 1  g ] (620 - 460 nm) and  1 A 1g  [b 2  2g ] →  1 E g  [b 1  2g  e 1  g ] (490 - 400 nm). The  3 E g  state is split by spin-orbit coupling into 5 components, from the one at lowest energy a luminescence emission (830 - 670 nm) takes place with a progression of 860 cm -1 , corresponding to the symmetric Os = O stretching vibration in the electronic ground state. The more intense bands are assigned to charge transfer transitions from oxo π-orbitals into unoccupied niveaus of Os (VI):  1 A 1g  [e 4  u ] →  3 A 2u  [e 3  u  e 1  g ] (390 - 340); →  1 A 1u  [e 3  u  e 1  g ] (340 - 290) and →  1 E u  [e 3  u  b 1  1g  (290 - 230 nm). The singlet-triplet distances are 3200-3600 cm  - 1 . From a Franck-Condon analysis an excited state elongation of 10-13 pm for the osmyl groups is calculated.

Die Schwingungsfeinstruktur der Elektronenspektren des 13 C- und 18 O-markierten trans-Dioxotetracyanoosmats (VI),[OsO 2 (CN) 4 ] 2 -