Open-shell solids exhibit ap lethora of intriguing physical phenomena that arise from ac omplex interplay of charge,s pin, orbital, and spin-state degrees of freedom. Comprehending these phenomena is an indispensable prerequisite for developing improved functional materials.T his type of understanding can be achieved, on the one hand, by experimental and theoretical investigations into knowns ystems,o rb ys ynthesizing new solids displaying unprecedented structural and/or electronic features. b-Ag 3 RuO 4 may serve as such amodel system because it possesses aremarkable anionic structure,c onsisting of tetrameric polyoxoanions (Ru 4 O 16 )
12À, and is an embedded fragment of a2Dtrigonal MO 2 lattice.The notorious frustration of antiferromagnetic (AF) exchange couplings on such lattices is thus lifted, and instead strong AF occurs within the oligomeric anion, where only one exchange path remains frustrated among the relevant six. The strong magnetic anisotropyo ft he [Ru 4 O 16 ] 12À ion, and the effectively orbital nature of its net magnetic moment, implies that this anion may reveal the properties of as ingle-molecule magnet if well-diluted in adiamagnetic matrix.Doubly negatively charged oxygen is unstable as afree ion, and thus it can only be incorporated into achemical environment if particular mechanisms of stabilization are enabled. An external positive potential provided by surrounding cations in ap revailingly ionic crystal is one of the most obvious options.[1] Another process giving relief to excess electron density is catenation with homo-atomic bonds, forming peroxide,s uperoxide,o ro zonide anions.[2] Forh igh oxidation state oxide materials,e lectron transfer to the coordinated cations commonly occurs within some kind of covalent bonding.T his feature of oxygen is one of the principal reasons for the tremendous wealth of structures and properties displayed by (multinary) oxides.A mong others, classes of materials include top performing ferroelectrics, [3] ferromagnets, [4] or superconductors.[5] Furthermore,s pecific charge,s pin, and orbital ordering phenomena give rise to aw ide-ranging spectrum of physical responses.S tructural variety is by no means al ess relevant factor,t ow hich the diversity of bulk properties of oxides can be related. For instance,a ntiferromagnetic exchange coupling of electron spins on atrigonal lattice is frustrated and raises arich energy landscape of ordered magnetic states.[6] Upon removal of part of the spin bearing species from such alattice (for example,by leaving behind aK agomØ-type pattern), frustrated magnetic exchange couplings may persist, while further breaking down the dimensionality leads to monomeric or oligomeric complex oxoanions,potentially behaving as single molecule magnets. [7] In particular, 2D trigonal lattices continue to be the focus of solid materials research, in combination with the phenomena of magnetic frustration and effects that are suited to lift the phenomenon.[6] Herein, we report on an ew oxoruthenate(V) featuring trigonal ...