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Functional molecule-based solids built of metal complexes can reveal a great impact of external stimuli upon their optical, magnetic, electric, and mechanical properties. We report a novel molecular material, {[Eu III (H 2 O) 3 (pyrone) 4 ][Co III (CN) 6 ]}· n H 2 O ( 1 , n = 2; 2 , n = 1), which was obtained by the self-assembly of Eu 3+ and [Co(CN) 6 ] 3- ions in the presence of a small 2-pyrrolidinone (pyrone) ligand in an aqueous medium. The as-synthesized material, 1 , consists of dinuclear cyanido-bridged {EuCo} molecules accompanied by two H-bonded water molecules. By lowering the relative humidity (RH) below 30% at room temperature, 1 undergoes a single-crystal-to-single-crystal transformation related to the partial removal of crystallization water molecules which results in the new crystalline phase, 2 . Both 1 and 2 solvates exhibit pronounced Eu III -centered visible photoluminescence. However, they differ in the energy splitting of the main emission band of a 5 D 0 → 7 F 2 origin, and the emission lifetime, which is longer in the partially dehydrated 2 . As the 1 ↔ 2 structural transformation can be repeatedly reversed by changing the RH value, the reported material shows a room-temperature switching of detailed luminescent features including the ratio between emission components and the emission lifetime values.

Reversible Humidity-Driven Transformation of a Bimetallic {EuCo} Molecular Material: Structural, Sorption, and Photoluminescence Studies