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The Jahn–Teller (JT) theorem constitutes one of the most fundamental concepts in chemistry. In transition‐element chemistry, the 3d 4  and 3d 9  configurations in octahedral complexes are particularly illustrative, where a distortion in local geometry is associated with a reduction of the electronic energy. However, there has been a lasting debate about the fact that the octahedra are found to exclusively elongate. In contrast, for Na 9 Bi 5 Os 3 O 24 , the octahedron around Os 6+ (5d 2 ) is heavily compressed, lifting the degeneracy of the  t 2g   set of 5 d  orbitals such that in the sense of a JT compression a diamagnetic ground state results. This effect is not forced by structural constraints, the structure offers sufficient space for osmium to shift the apical oxygen atoms to a standard distance. The relevance of these findings is far reaching, since they provide new insights in the hierarchy of perturbations defining ground states of open shell electronic systems.

Na 9 Bi 5 Os 3 O 24 : A Diamagnetic Oxide Featuring a Pronouncedly Jahn–Teller‐Compressed Octahedral Coordination of Osmium(VI)